253 results on '"Gong, Jinlong"'
Search Results
2. Reversed Electron Transfer in Dual Single Atom Catalyst for Boosted Photoreduction of CO2.
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Zhang, Yanzhao, Johannessen, Bernt, Zhang, Peng, Gong, Jinlong, Ran, Jingrun, and Qiao, Shi‐Zhang
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- 2023
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3. Fast‐Response Nickel‐Promoted Indium Oxide Catalysts for Carbon Dioxide Hydrogenation from Intermittent Solar Hydrogen.
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Li, Xianghong, Zhang, Peng, Yang, Chengsheng, Wang, Zhongyan, Song, Xiwen, Wang, Tuo, and Gong, Jinlong
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INDIUM oxide ,CARBON dioxide ,WATER electrolysis ,GREENHOUSE effect ,CATALYST structure ,HYDROGENATION ,INTERSTITIAL hydrogen generation - Abstract
Construction of a "net‐zero‐emission" system through CO2 hydrogenation to methanol with solar energy is an eco‐friendly way to mitigate the greenhouse effect. Traditional CO2 hydrogenation demands centralized mass production for cost reduction with mass water electrolysis for hydrogen supply. To achieve continuous reaction with intermittent and fluctuating flow of H2 on a small‐scale for distributed application scenarios, modulating the catalyst interface environment and chemical adsorption capacity to adapt fluctuating reaction conditions is highly desired. This paper describes a distributed clean CO2 utilization system in which the surface structure of catalysts is carefully regulated. The Ni catalyst with unsaturated electrons loaded on In2O3 can reduce the dissociation energy of H2 to overcome the slow response of intermittent H2 supply, exhibiting a faster response (12 min) than bare oxide catalysts (42 min). Moreover, the introduction of Ni enhances the sensitivity of the catalyst to hydrogen, yielding a Ni/In2O3 catalyst with a good performance at lower H2 concentrations with a 15 times adaptability for wider hydrogen fluctuation range than In2O3, greatly reducing the negative impact of unstable H2 supplies derived from renewable energies. [ABSTRACT FROM AUTHOR]
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- 2023
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4. High‐Throughput Screening of Electrocatalysts for Nitrogen Reduction Reactions Accelerated by Interpretable Intrinsic Descriptor.
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Lin, Xiaoyun, Wang, Yongtao, Chang, Xin, Zhen, Shiyu, Zhao, Zhi‐Jian, and Gong, Jinlong
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HIGH throughput screening (Drug development) ,ELECTROCATALYSTS ,STRUCTURE-activity relationships ,MOLECULAR orbitals ,TRANSITION metals ,OXYGEN reduction ,NITROGEN ,ELECTROLYTIC reduction - Abstract
Developing easily accessible descriptors is crucial but challenging to rationally design single‐atom catalysts (SACs). This paper describes a simple and interpretable activity descriptor, which is easily obtained from the atomic databases. The defined descriptor proves to accelerate high‐throughput screening of more than 700 graphene‐based SACs without computations, universal for 3–5d transition metals and C/N/P/B/O‐based coordination environments. Meanwhile, the analytical formula of this descriptor reveals the structure–activity relationship at the molecular orbital level. Using electrochemical nitrogen reduction as an example, this descriptor's guidance role has been experimentally validated by 13 previous reports as well as our synthesized 4 SACs. Orderly combining machine learning with physical insights, this work provides a new generalized strategy for low‐cost high‐throughput screening while comprehensive understanding the structure‐mechanism‐activity relationship. [ABSTRACT FROM AUTHOR]
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- 2023
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5. Data‐Driven Interpretable Descriptors for the Structure–Activity Relationship of Surface Lattice Oxygen on Doped Vanadium Oxides.
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Jiang, Chenggong, Song, Hongbo, Sun, Guodong, Chang, Xin, Zhen, Shiyu, Wu, Shican, Zhao, Zhi‐Jian, and Gong, Jinlong
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STRUCTURE-activity relationships ,VANADIUM oxide ,CHEMICAL-looping combustion ,OXIDATIVE dehydrogenation ,DENSITY functional theory ,OXYGEN ,OXIDATIVE addition ,OXYGEN reduction - Abstract
Understanding the structure–activity relationship of surface lattice oxygen is critical but challenging to design efficient redox catalysts. This paper describes data‐driven redox activity descriptors on doped vanadium oxides combining density functional theory and interpretable machine learning. We corroborate that the p‐band center is the most crucial feature for the activity. Besides, some features from the coordination environment, including unoccupied d‐band center, s‐ and d‐band fillings, also play important roles in tuning the oxygen activity. Further analysis reveals that data‐driven descriptors could decode more information about electron transfer during the redox process. Based on the descriptors, we report that atomic Re‐ and W‐doping could inhibit over‐oxidation in the chemical looping oxidative dehydrogenation of propane, which is verified by subsequent experiments and calculations. This work sheds light on the structure–activity relationship of lattice oxygen for the rational design of redox catalysts. [ABSTRACT FROM AUTHOR]
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- 2022
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6. Synergistic Mechanism of Platinum‐GaOx Catalysts for Propane Dehydrogenation.
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Zhang, Tingting, Pei, Chunlei, Sun, Guodong, Chen, Sai, Zhao, Zhi‐Jian, Sun, Shijia, Lu, Zhenpu, Xu, Yiyi, and Gong, Jinlong
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DEHYDROGENATION ,PROPANE ,GALLIUM alloys ,METALLIC oxides ,CATALYSTS ,PROPENE - Abstract
The synergy between metals and metal oxides can effectively improve the heterogeneous catalytic process. This paper describes the intrinsic effect of Pt modification over GaOx (Pt−GaOx) on propane dehydrogenation. The presence of Pt promotes H2 dissociation and surface coverage of hydrogen species, which is beneficial for the activation of C−H in propane. With excessive Pt, Gaδ+ can be further reduced to form Pt−Ga alloy with less surface hydrogen species. Consequently, the relative propylene formation rate between Pt−GaOx and the summed contribution of individual Pt and GaOx increases linearly with the content of hydrogen species. Optimally, the relative propylene formation rate of Pt−GaOx with 0.03 wt % Pt exceeds 25 % of the summed contribution of individual components. [ABSTRACT FROM AUTHOR]
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- 2022
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7. A Transparent, High‐Performance, and Stable Sb2S3 Photoanode Enabled by Heterojunction Engineering with Conjugated Polycarbazole Frameworks for Unbiased Photoelectrochemical Overall Water Splitting Devices.
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Wang, Lei, Lian, Weitao, Liu, Bin, Lv, Haifeng, Zhang, Ying, Wu, Xiaojun, Wang, Tuo, Gong, Jinlong, Chen, Tao, and Xu, Hangxun
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- 2022
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8. Nature of the Active Sites of Copper Zinc Catalysts for Carbon Dioxide Electroreduction.
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Zhen, Shiyu, Zhang, Gong, Cheng, Dongfang, Gao, Hui, Li, Lulu, Lin, Xiaoyun, Ding, Zheyuan, Zhao, Zhi‐Jian, and Gong, Jinlong
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ZINC catalysts ,COPPER catalysts ,CARBON dioxide ,HIGH throughput screening (Drug development) ,COUPLING reactions (Chemistry) ,ELECTROLYTIC reduction - Abstract
The electrochemical CO2 reduction (CO2ER) to multi‐carbon chemical feedstocks over Cu‐based catalysts is of considerable attraction but suffers with the ambiguous nature of active sites, which hinder the rational design of catalysts and large‐scale industrialization. This paper describes a large‐scale simulation to obtain realistic CuZn nanoparticle models and the atom‐level structure of active sites for C2+ products on CuZn catalysts in CO2ER, combining neural network based global optimization and density functional theory calculations. Upon analyzing over 2000 surface sites through high throughput tests based on NN potential, two kinds of active sites are identified, balanced Cu−Zn sites and Zn‐heavy Cu−Zn sites, both facilitating C−C coupling, which are verified by subsequent calculational and experimental investigations. This work provides a paradigm for the design of high‐performance Cu‐based catalysts and may offer a general strategy to identify accurately the atomic structures of active sites in complex catalytic systems. [ABSTRACT FROM AUTHOR]
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- 2022
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9. Enabling High Loading in Single‐Atom Catalysts on Bare Substrate with Chemical Scissors by Saturating the Anchoring Sites.
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Li, Ang, Kan, Erjun, Chen, Shuangming, Du, Zhengwei, Liu, Xuan, Wang, Tongyu, Zhu, Wenjin, Huo, Hailing, Ma, Jingjing, Liu, Dong, Song, Li, Feng, Hao, Antonietti, Markus, and Gong, Jinlong
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- 2022
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10. Moderate Surface Segregation Promotes Selective Ethanol Production in CO2 Hydrogenation Reaction over CoCu Catalysts.
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Liu, Sihang, Yang, Chengsheng, Zha, Shenjun, Sharapa, Dmitry, Studt, Felix, Zhao, Zhi‐Jian, and Gong, Jinlong
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SURFACE segregation ,CATALYSTS ,ETHANOL ,HYDROGENATION ,INDUSTRIAL capacity ,SURFACE morphology ,CARBON dioxide - Abstract
Cobalt‐copper (CoCu) catalysts have industrial potential in CO/CO2 hydrogenation reactions, and CoCu alloy has been elucidated as a major active phase during reactions. However, due to elemental surface segregation and dealloying phenomena, the actual surface morphology of CoCu alloy is still unclear. Combining theory and experiment, the dual effect of surface segregation and varied CO coverage over the CoCu(111) surface on the reactivity in CO2 hydrogenation reactions is explored. The relationship between C−O bond scission and further hydrogenation of intermediate *CH2O was discovered to be a key step to promote ethanol production. The theoretical investigation suggests that moderate Co segregation provides a suitable surface Co ensemble with lateral interactions of co‐adsorbed *CO, leading to promoted selectivity to ethanol, in agreement with theory‐inspired experiments. [ABSTRACT FROM AUTHOR]
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- 2022
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11. Pt–Cu Interaction Induced Construction of Single Pt Sites for Synchronous Electron Capture and Transfer in Photocatalysis.
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Su, Lina, Wang, Pengfei, Wang, Junhui, Zhang, Dongpeng, Wang, Haitao, Li, Yi, Zhan, Sihui, and Gong, Jinlong
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ELECTRON capture ,CHARGE exchange ,DIFFUSION barriers ,CHARGE transfer ,DENSITY functional theory ,HYDROGEN evolution reactions ,PHOTOCATALYSIS - Abstract
Single‐atom photocatalysts have shown their fascinating strengths in enhancing charge transfer dynamics; however, rationally designing coordination sites by metal doping to stabilize isolated atoms is still challenging. Here, a one‐unit‐cell ZnIn2S4 (ZIS) nanosheet with abundant Cu dopants serving as the suitable support to achieve a single atom Pt catalyst (Pt1/Cu–ZIS) is reported, and hence the metal single atom–metal dopant interaction at an atomic level is disclosed. Experimental results and density functional theory calculations highlight the unique stabilizing effect (Pt–Cu interaction) of single Pt atoms in Cu‐doped ZIS, while apparent Pt clusters are observed in pristine ZIS. Specifically, Pt–Cu interaction provides an extra coordination site except three S sites on the surface, which induces a higher diffusion barrier and makes the single atom more stable on the surface. Apart from stabilizing Pt single atoms, Pt–Cu interaction also serves as the efficient channel to transfer electrons from Cu trap states to Pt active sites, thereby enhancing the charge separation and transfer efficiency. Remarkably, the Pt1/Cu–ZIS exhibits a superb activity, giving a photocatalytic hydrogen evolution rate of 5.02 mmol g−1 h−1, nearly 49 times higher than that of pristine ZIS. [ABSTRACT FROM AUTHOR]
- Published
- 2021
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12. Controllable Cu0‐Cu+ Sites for Electrocatalytic Reduction of Carbon Dioxide.
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Yuan, Xintong, Chen, Sai, Cheng, Dongfang, Li, Lulu, Zhu, Wenjin, Zhong, Dazhong, Zhao, Zhi‐Jian, Li, Jingkun, Wang, Tuo, and Gong, Jinlong
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CARBON dioxide reduction ,ELECTROLYTIC reduction ,COUPLING reactions (Chemistry) ,STANDARD hydrogen electrode ,DENSITY functional theory ,CHARGE exchange - Abstract
Cu‐based electrocatalysts facilitate CO2 electrochemical reduction (CO2ER) to produce multi‐carbon products. However, the roles of Cu0 and Cu+ and the mechanistic understanding remain elusive. This paper describes the controllable construction of Cu0‐Cu+ sites derived from the well‐dispersed cupric oxide particles supported on copper phyllosilicate lamella to enhance CO2ER performance. 20 % Cu/CuSiO3 shows the superior CO2ER performance with 51.8 % C2H4 Faraday efficiency at −1.1 V vs reversible hydrogen electrode during the 6 hour test. In situ attenuated total reflection infrared spectra and density functional theory (DFT) calculations were employed to elucidate the reaction mechanism. The enhancement in CO2ER activity is mainly attributed to the synergism of Cu0‐Cu+ pairs: Cu0 activates CO2 and facilitates the following electron transfers; Cu+ strengthens *CO adsorption to further boost C−C coupling. We provide a strategy to rationally design Cu‐based catalysts with viable valence states to boost CO2ER. [ABSTRACT FROM AUTHOR]
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- 2021
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13. Arificial Leaves for Solar Fuels.
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Zhang, Gong Please check if link to ORCID is correct. --> Please confirm that given names (blue) and surnames/family names (vermilion) have been identified correctly. -->, Liu, Bin, Wang, Tuo, and Gong, Jinlong
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HYDROGEN as fuel ,ENERGY consumption ,FOSSIL fuels ,ARTIFICIAL photosynthesis ,ELECTROLYTIC reduction ,METHANOL as fuel ,SOLAR energy - Abstract
Large amounts of anthropogenic CO2 emissions associated with increased fossil fuel consumption have led to global warming. Upgrading CO2 and water into solar fuels such as hydrogen, methanol, ethanol, etc., is believed to be one of the best methods to address this serious problem. Herein, we focus on introducing our endeavor of developing the photoelectrochemical water splitting reaction system, constructing the (photo)electrochemical CO2 reduction reaction system, and realizing the artificial leaves. This paper consists of a brief introduction, representative applications, and related mechanisms. These research results would be helpful to achieve sustainable development in our society based on the use of solar energy. What is the most important personality for scientific research? Courage and perseverance to overcome difficulties in new research fields. Who influences you mostly in your life? George M. Whitesides. What is the most favorite and original chemistry developed in your research group? Regulating electronic structure and defects of catalysts for artificial photosynthesis. How do you supervise your students? Share the latest research results with students and discuss with them frequently to help them develop their scientific skills. How do you keep balance between research and family? Organize and plan ahead of time. Make flexible schedules. What are your hobbies? Hiking and swimming. [ABSTRACT FROM AUTHOR]
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- 2021
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14. Coupling of Cu(100) and (110) Facets Promotes Carbon Dioxide Conversion to Hydrocarbons and Alcohols.
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Zhong, Dazhong, Zhao, Zhi‐Jian, Zhao, Qiang, Cheng, Dongfang, Liu, Bin, Zhang, Gong, Deng, Wanyu, Dong, Hao, Zhang, Lei, Li, Jingkun, Li, Jinping, and Gong, Jinlong
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CARBON dioxide ,CARBON dioxide reduction ,COUPLING reactions (Chemistry) ,COPPER crystals ,STANDARD hydrogen electrode ,OXAZOLIDINONES - Abstract
Copper can efficiently electro‐catalyze carbon dioxide reduction to C2+ products (C2H4, C2H5OH, n‐propanol). However, the correlation between the activity and active sites remains ambiguous, impeding further improvements in their performance. The facet effect of copper crystals to promote CO adsorption and C−C coupling and consequently yield a superior selectivity for C2+ products is described. We achieve a high Faradaic efficiency (FE) of 87 % and a large partial current density of 217 mA cm−2 toward C2+ products on Cu(OH)2‐D at only −0.54 V versus the reversible hydrogen electrode in a flow‐cell electrolyzer. With further coupled to a Si solar cell, record‐high solar conversion efficiencies of 4.47 % and 6.4 % are achieved for C2H4 and C2+ products, respectively. This study provides an in‐depth understanding of the selective formation of C2+ products on Cu and paves the way for the practical application of electrocatalytic or solar‐driven CO2 reduction. [ABSTRACT FROM AUTHOR]
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- 2021
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15. Controllable Distribution of Oxygen Vacancies in Grain Boundaries of p‐Si/TiO2 Heterojunction Photocathodes for Solar Water Splitting.
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Li, Huimin, Wang, Tuo, Liu, Shanshan, Luo, Zhibin, Li, Lulu, Wang, Huaiyuan, Zhao, Zhi‐Jian, and Gong, Jinlong
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PHOTOCATHODES ,CRYSTAL grain boundaries ,HETEROJUNCTIONS ,OXYGEN ,AQUEOUS electrolytes ,SILICON solar cells ,HYDROGEN production - Abstract
Silicon is a promising photocathode material in photoelectrochemical water splitting for hydrogen production, but it is primarily limited by photocorrosion in aqueous electrolytes. As an extensively used protective material, crystalline TiO2 could protect Si photoelectrode against corrosion. However, a large number of grain boundaries (GBs) in polycrystalline TiO2 would induce excessive recombination centers, impeding the carrier transport. This paper describes the introduction of oxygen vacancies (Ovac) with controllable spatial distribution for GBs to promote carrier transport. Two kinds of Ovac distribution, Ovac along GBs and Ovac inside grains, are compared, where the latter one is demonstrated to facilitate carrier transport owing to the formation of tunneling paths across GBs. Consequently, a simple p‐Si/TiO2/Pt heterojunction photocathode with controllable Ovac distribution in TiO2 shows a +400 mV onset potential shift and yields an applied bias photon‐to‐current efficiency of 5.9 %, which is the best efficiency reported among silicon photocathodes except for silicon homojunction. [ABSTRACT FROM AUTHOR]
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- 2021
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16. Double‐Side Si Photoelectrode Enabled by Chemical Passivation for Photoelectrochemical Hydrogen and Oxygen Evolution Reactions.
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Liu, Bin, Wang, Shujie, Feng, Shijia, Li, He, Yang, Lifei, Wang, Tuo, and Gong, Jinlong
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OXYGEN evolution reactions ,HYDROGEN evolution reactions ,PASSIVATION ,CHARGE carrier lifetime ,PHOTOELECTROCHEMICAL cells ,SURFACE passivation ,OXIDATION of water - Abstract
This paper describes a Si photoelectrode with an ultra‐long minority carrier diffusion length (1940 µm) passivated by an amorphous Si layer, which provides a chemically passivated surface. With this extremely long carrier diffusion length, it is possible to separate the catalyst layer (metal) with the light absorption region on different sides of the Si photoelectrode, forming a double‐side Si photoelectrode for photoelectrochemical water reduction and oxidation. The obtained photocathode exhibits a photocurrent of 39 mA cm−2 and applied bias photon‐to‐current efficiencies (ABPE) of 15.4% with stability up to 100 h. Meanwhile, 38.5 mA cm−2 photocurrent and ABPE of 5.8% with a 200 h stability are achieved when this structure is used as a photoanode. A monolithic unbiased artificial leaf is constructed, yielding an unbiased solar to hydrogen conversion efficiency of 3.7%. This chemically passivated Si photoelectrode breaks the trade‐off between carrier transport and surface passivation in conventional Si photoelectrodes. [ABSTRACT FROM AUTHOR]
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- 2021
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17. Selective Electroreduction of Carbon Dioxide over SnO2‐Nanodot Catalysts.
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Hu, Congling, Li, Lulu, Deng, Wanyu, Zhang, Gong, Zhu, Wenjin, Yuan, Xintong, Zhang, Lei, Zhao, Zhi‐Jian, and Gong, Jinlong
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OXYGEN evolution reactions ,ELECTROLYTIC reduction ,OVERPOTENTIAL ,ENERGY consumption ,CARBON dioxide - Abstract
The development of electrochemical CO2 conversion allows green carbon utilization. Formate and syngas are two typical products of electrochemical CO2 reduction, and the coproduction of these two products will maximize the energy efficiency of CO2 conversion. However, few works have successfully achieved the cogeneration of formate and syngas. This paper describes a novel strategy to maximize the efficiency of CO2 conversion through coproduction of formate and syngas on ultrasmall SnO2 nanodots (NDs) homogeneously anchored on carbon nanotubes (CNT#SnO2 NDs) electrodes. The CNT#SnO2 NDs not only decreased the adsorption energy of *OCHO but also reduced the adsorption energy difference of *COOH and *H. High energy efficiency toward formate and adjustable H2/CO ratio were obtained over a broad potential window with long‐term stability. In addition, CNT#SnO2 NDs and Ir foil were coupled together to construct an electrolyzer for electrochemical CO2 reduction reaction and oxygen evolution reaction (CO2ERR–OER), which also produced formate and syngas with 24 h stability. A promising approach is presented for the electrochemical CO2 conversion in fuel production. [ABSTRACT FROM AUTHOR]
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- 2020
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18. Coverage‐Dependent Behaviors of Vanadium Oxides for Chemical Looping Oxidative Dehydrogenation.
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Chen, Sai, Pei, Chunlei, Chang, Xin, Zhao, Zhi‐Jian, Mu, Rentao, Xu, Yiyi, and Gong, Jinlong
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OXIDATIVE dehydrogenation ,VANADIUM oxide ,CHEMICAL-looping combustion ,CATALYTIC dehydrogenation ,CHEMICAL reactions ,KIRKENDALL effect ,CARBON dioxide - Abstract
Chemical looping provides an energy‐ and cost‐effective route for alkane utilization. However, there is considerable CO2 co‐production caused by kinetically mismatched O2− bulk diffusion and surface reaction in current chemical looping oxidative dehydrogenation systems, rendering a decreased olefin productivity. Sub‐monolayer or monolayer vanadia nanostructures are successfully constructed to suppress CO2 production in oxidative dehydrogenation of propane by evading the interference of O2− bulk diffusion (monolayer versus multi‐layers). The highly dispersed vanadia nanostructures on titanium dioxide support showed over 90 % propylene selectivity at 500 °C, exhibiting turnover frequency of 1.9×10−2 s−1, which is over 20 times greater than that of conventional crystalline V2O5. Combining in situ spectroscopic characterizations and DFT calculations, we reveal the loading–reaction barrier relationship through the vanadia/titanium interfacial interaction. [ABSTRACT FROM AUTHOR]
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- 2020
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19. Enhanced CO2 Electroreduction on Neighboring Zn/Co Monomers by Electronic Effect.
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Zhu, Wenjin, Zhang, Lei, Liu, Sihang, Li, Ang, Yuan, Xintong, Hu, Congling, Zhang, Gong, Deng, Wanyu, Zang, Ketao, Luo, Jun, Zhu, Yuanmin, Gu, Meng, Zhao, Zhi‐Jian, and Gong, Jinlong
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POLAR effects (Chemistry) ,EXTENDED X-ray absorption fine structure ,ELECTROLYTIC reduction ,MONOMERS ,METAL-metal bonds ,ELECTRONIC paper ,CARBON dioxide reduction - Abstract
It is of great significance to reveal the detailed mechanism of neighboring effects between monomers, as they could not only affect the intermediate bonding but also change the reaction pathway. This paper describes the electronic effect between neighboring Zn/Co monomers effectively promoting CO2 electroreduction to CO. Zn and Co atoms coordinated on N doped carbon (ZnCoNC) show a CO faradaic efficiency of 93.2 % at −0.5 V versus RHE during a 30‐hours test. Extended X‐ray absorption fine structure measurements (EXAFS) indicated no direct metal–metal bonding and X‐ray absorption near‐edge structure (XANES) showed the electronic effect between Zn/Co monomers. In situ attenuated total reflection‐infrared spectroscopy (ATR‐IR) and density functional theory (DFT) calculations further revealed that the electronic effect between Zn/Co enhanced the *COOH intermediate bonding on Zn sites and thus promoted CO production. This work could act as a promising way to reveal the mechanism of neighboring monomers and to influence catalysis. [ABSTRACT FROM AUTHOR]
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- 2020
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20. A novel impedance adapter for the time‐domain electromagnetic pulse standard field generation setup.
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Wang, Yifan, Gong, Jinlong, Yang, Qing, and Huang, Hui
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ELECTROMAGNETIC pulses , *SIGNAL generators , *INSERTION loss (Telecommunication) , *NATIONAL competency-based educational tests , *ABSORPTION of sound , *WORK design - Abstract
The purpose of the work is to design a novel impedance adapter to set up a mono‐cone standard field generation system with a large clear time and a large dynamic range. To transform the impedance from 50 Ω (the output impedance of the signal generator) to 75 Ω (the input impedance of the cone), the gradient structures with 11 sections are designed for the impedance adapter. The measured VSWR of the system is below 1.5 from 300 to 2.25 GHz. The insertion loss of the designed is about −35 dB. The system with the designed impedance adapter works well. This is validated by the results of the standard open‐air test site in National Institute of Metrology, China. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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21. Enriched Surface Oxygen Vacancies of Photoanodes by Photoetching with Enhanced Charge Separation.
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Feng, Shijia, Wang, Tuo, Liu, Bin, Hu, Congling, Li, Lulu, Zhao, Zhi‐Jian, and Gong, Jinlong
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PHOTOCATHODES ,STANDARD hydrogen electrode ,DENSITY functional theory ,OXYGEN ,OXIDATION of water - Abstract
A facile photoetching approach is described that alleviates the negative effects from bulk defects by confining the oxygen vacancy (Ovac) at the surface of BiVO4 photoanode, by 10‐minute photoetching. This strategy could induce enriched Ovac at the surface of BiVO4, which avoids the formation of excessive bulk defects. A mechanism is proposed to explain the enhanced charge separation at the BiVO4 /electrolyte interface, which is supported by density functional theory (DFT) calculations. The optimized BiVO4 with enriched surface Ovac presents the highest photocurrent among undoped BiVO4 photoanodes. Upon loading FeOOH/NiOOH cocatalysts, photoetched BiVO4 photoanode reaches a considerable water oxidation photocurrent of 3.0 mA cm−2 at 0.6 V vs. reversible hydrogen electrode. An unbiased solar‐to‐hydrogen conversion efficiency of 3.5 % is realized by this BiVO4 photoanode and a Si photocathode under 1 sun illumination. [ABSTRACT FROM AUTHOR]
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- 2020
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22. Three‐Phase Photocatalysis for the Enhanced Selectivity and Activity of CO2 Reduction on a Hydrophobic Surface.
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Li, Ang, Cao, Qian, Zhou, Guangye, Schmidt, Bernhard V. K. J., Zhu, Wenjin, Yuan, Xintong, Huo, Hailing, Gong, Jinlong, and Antonietti, Markus
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HYDROPHOBIC surfaces ,PHOTOCATALYSIS ,HYDROGEN evolution reactions ,PHOTOREDUCTION ,PLATINUM nanoparticles ,RENEWABLE natural resources ,AQUEOUS solutions - Abstract
The photocatalytic CO2 reduction reaction (CRR) represents a promising route for the clean utilization of stranded renewable resources, but poor selectivity resulting from the competing hydrogen evolution reaction (HER) in aqueous solution limits its practical applicability. In the present contribution a photocatalyst with hydrophobic surfaces was fabricated. It facilitates an efficient three‐phase contact of CO2 (gas), H2O (liquid), and catalyst (solid). Thus, concentrated CO2 molecules in the gas phase contact the catalyst surface directly, and can overcome the mass‐transfer limitations of CO2, inhibit the HER because of lowering proton contacts, and overall enhance the CRR. Even when loaded with platinum nanoparticles, one of the most efficient HER promotion cocatalysts, the three‐phase photocatalyst maintains a selectivity of 87.9 %. Overall, three‐phase photocatalysis provides a general and reliable method to enhance the competitiveness of the CRR. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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23. The Interplay between Structure and Product Selectivity of CO2 Hydrogenation.
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Yang, Chengsheng, Liu, Sihang, Wang, Yanan, Song, Jimin, Wang, Guishuo, Wang, Shuai, Zhao, Zhi‐Jian, Mu, Rentao, and Gong, Jinlong
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HYDROGENATION ,HETEROGENEOUS catalysts ,METHANATION ,SURFACE structure ,NANORODS ,MANUFACTURED products - Abstract
Identification of the active structure under reaction conditions is of great importance for the rational design of heterogeneous catalysts. However, this is often hampered by their structural complexity. The interplay between the surface structure of Co3O4 and the CO2 hydrogenation is described. Co3O4 with morphology‐dependent crystallographic surfaces presents different reducibility and formation energy of oxygen vacancies, thus resulting in distinct steady‐state composition and product selectivity. Co3O4‐0 h rhombic dodecahedra were completely reduced to Co0 and CoO, which presents circa 85 % CH4 selectivity. In contrast, Co3O4‐2 h nanorods were partially reduced to CoO, which exhibits a circa 95 % CO selectivity. The crucial role of the Co3O4 structure in determining the catalytic performance for higher alcohol synthesis over CuCo‐based catalysts is demonstrated. As expected, Cu/Co3O4‐2 h shows nine‐fold higher ethanol yield than Cu/Co3O4‐0 h owing to the inhibition for methanation. [ABSTRACT FROM AUTHOR]
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- 2019
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24. Broadband Light Harvesting and Unidirectional Electron Flow for Efficient Electron Accumulation for Hydrogen Generation.
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Zhang, Nan, Qi, Ming‐Yu, Yuan, Lan, Fu, Xianzhi, Tang, Zi‐Rong, Gong, Jinlong, and Xu, Yi‐Jun
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HYDROGEN evolution reactions ,PLATINUM nanoparticles ,INTERSTITIAL hydrogen generation ,HOT carriers ,ELECTRONS ,ATOMIC hydrogen ,CHARGE exchange - Abstract
The efficiency of solar hydrogen evolution closely depends on the multiple electrons accumulation on the catalytic center for two‐electron‐involved water reduction. Herein, we report an effective approach to enable broadband light absorption and unidirectional electron flow for efficiently accumulating electrons at active sites for hydrogen evolution by rationally engineering the nanostructure of Pt nanoparticles (NPs), TiO2, and SiO2 support. In addition to Schottky‐junction‐driven electron transfer from TiO2 to Pt, Pt NPs also produce hot electrons by recycling the scattered visible and near‐infrared (vis‐NIR) light of the support. Unidirectional electron flow to active sites is realized by tuning the components spatial distribution. These features collectively accumulate multiple electrons at catalytic Pt sites, thereby affording enhanced activity toward hydrogen evolution under simulated sunlight. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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25. Activation and Spillover of Hydrogen on Sub‐1 nm Palladium Nanoclusters Confined within Sodalite Zeolite for the Semi‐Hydrogenation of Alkynes.
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Wang, Shuai, Zhao, Zhi‐Jian, Chang, Xin, Zhao, Jiubing, Tian, Hao, Yang, Chengsheng, Li, Mingrun, Fu, Qiang, Mu, Rentao, and Gong, Jinlong
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SODALITE ,HYDROXYL group ,ALKYNES ,HYDROGEN atom ,PALLADIUM ,HYDROGEN - Abstract
The search for efficient nontoxic catalysts able to perform industrial hydrogenations is a topic of interest, with relevance to many catalytic processes. Herein, we describe a mechanistic phenomenon for the activation and spillover of hydrogen for remarkable selectivity in the semi‐hydrogenation of acetylene over sub‐1 nm Pd nanoclusters confined within sodalite (SOD) zeolite (Pd@SOD). Specifically, hydrogen is dissociated on the Pd nanoclusters to form hydrogen species (i.e., hydrogen atoms and hydroxyl groups) that spill over the SOD surfaces. The design and utilization of the small‐pore zeolite SOD (six‐membered rings with 0.28×0.28 nm channels) is crucial as it only allows H2 diffusion into the channels to reach the encapsulated Pd nanoclusters and thus avoids over‐hydrogenation to form ethane. Pd@SOD exhibits an ethylene selectivity of over 94.5 %, while that of conventional Pd/SOD is approximately 21.5 %. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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- View/download PDF
26. Nanopolyaniline Coupled with an Anticorrosive Graphene as a 3D Film Electrocatalyst for Efficient Oxidation of Toluene Methyl C−H Bonds and Hydrogen Production at Low Voltage.
- Author
-
Zhu, Yanji, Wang, Huaiyuan, Jin, Kai, and Gong, Jinlong
- Subjects
OXIDATION of toluene ,HYDROGEN production ,3-D films ,LOW voltage systems ,HYDROGEN bonding ,INTERSTITIAL hydrogen generation ,CHEMICAL bonds - Abstract
A graphene‐wrapped polyaniline nanoparticles film embedded in carbon cloth (CC/PANI/G) was fabricated and used as a 3D anodic electrocatalyst for oxidation of toluene methyl C−H groups. The methyl C−H bonds can be oxidized effectively at the CC/PANI/G anode with 99.9 % toluene conversion at a low applied voltage of only 1.0 V, which implies low energy input. Importantly, 86.6 % of toluene methyl C−H groups were converted to benzoyl groups (C=O), and hydrogen was produced efficiently at the cathode. The electrocatalytic efficiency at the CC/PANI/G anode was higher at lower voltage (1.0 V) than at higher voltage (1.5 V), and more hydrogen was produced at the corresponding cathode. The synergistic effect between the dynamic redox chemistry of nanoPANI and the excellent conductivity and anticorrosive action of graphene determined the high electrocatalytic efficiency of the oxidation of toluene methyl C−H groups at the CC/PANI/G anode. Owing to the chemical bonding between graphene and PANI, the anticorrosive CC/PANI/G anodic electrocatalyst was durable and effective for oxidation of toluene methyl C−H groups in acidic environment. This approach provides advanced electrode materials for transforming stable chemical bonds (C−H) into useful functional groups (C=O), which will be beneficial for the synthesis of organic intermediates with coupled hydrogen production. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
27. Adjusting the Reduction Potential of Electrons by Quantum Confinement for Selective Photoreduction of CO2 to Methanol.
- Author
-
Li, Ang, Wang, Tuo, Li, Chengcheng, Huang, Zhiqi, Luo, Zhibin, and Gong, Jinlong
- Subjects
POLYMERIC nanocomposites ,REDUCTION potential ,HYDROGEN evolution reactions ,ELECTRONS - Abstract
The production of CH3OH from the photocatalytic CO2 reduction reaction (PCRR) presents a promising route for the clean utilization of renewable resources, but charge recombination, an unsatisfying stability and a poor selectivity limit its practical application. In this paper, we present the design and fabrication of 0D/2D materials with polymeric C3N4 nanosheets and CdSe quantum dots (QDs) to enhance the separation and reduce the diffusion length of charge carriers. The rapid outflow of carriers also restrains self‐corrosion and consequently enhances the stability. Furthermore, based on quantum confinement effects of the QDs, the energy of the electrons could be adjusted to a level that inhibits the hydrogen evolution reaction (HER, the main competitive reaction to PCRR) and improves the selectivity and activity for CH3OH production from the PCRR. The band structures of photocatalysts with various CdSe particle sizes were also investigated quantitatively to establish the relationship between the band energy and the photocatalytic performance. Reduced to the max: A strategy for selective photocatalytic CO2 reduction in aqueous solution based on the adjustment of the reduction potential of electrons in CdSe quantum dots is presented. The approach also inhibits the competitive hydrogen evolution reaction. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
28. Competition of C‐C bond formation and C‐H bond formation For acetylene hydrogenation on transition metals: A density functional theory study.
- Author
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Zhao, Zhi‐Jian, Zhao, Jiubing, Chang, Xin, Zha, Shenjun, Zeng, Liang, and Gong, Jinlong
- Subjects
CARBON-hydrogen bonds ,DENSITY functional theory ,COUPLING reactions (Chemistry) ,HYDROGENATION ,ETHYLENE - Abstract
Selective hydrogenation of acetylene is an important reaction for production of polymer grade ethylene. The green oil formation has great influence on the selectivity and activity of acetylene selective hydrogenation. This article describes a density functional theory study on the C + H hydrogenation reaction and C + C coupling reaction on the (111) surface of Ag, Cu, Pd, Pt, Rh, and Ir. The activity of acetylene selective hydrogenation is examined by the effective barrier for ethylene formation. A comparison between the reaction barrier of ethylene hydrogenation and desorption is used to identify the selectivity for ethylene formation. The barriers of three pathways for 1,3‐butadiene formation suggest that acetylene and vinyl coupling reaction is the favorable pathway. The stability of catalysts is evaluated by the selectivity of 1,3‐butadiene, which follows the order of Pt(111) > Ir(111) > Rh(111) > Pd(111) > Cu(111) > Ag(111). Furthermore, the relationship between acetylene adsorption energy and effective barrier of ethylene formation and 1,3‐butadiene formation has been established to well understand the catalytic properties of different metals. © 2018 American Institute of Chemical Engineers AIChE J, 65: 1059–1066, 2019 [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
29. Tuning Cu/Cu2O Interfaces for the Reduction of Carbon Dioxide to Methanol in Aqueous Solutions.
- Author
-
Chang, Xiaoxia, Wang, Tuo, Zhao, Zhi‐Jian, Yang, Piaoping, Greeley, Jeffrey, Mu, Rentao, Zhang, Gong, Gong, Zhongmiao, Luo, Zhibin, Chen, Jun, Cui, Yi, Ozin, Geoffrey A., and Gong, Jinlong
- Subjects
CARBON dioxide ,AQUEOUS solutions ,METHANOL ,ARTIFICIAL photosynthesis ,COPPER ,NANOPARTICLES ,ELECTROLYTES - Abstract
Artificial photosynthesis can be used to store solar energy and reduce CO2 into fuels to potentially alleviate global warming and the energy crisis. Compared to the generation of gaseous products, it remains a great challenge to tune the product distribution of artificial photosynthesis to liquid fuels, such as CH3OH, which are suitable for storage and transport. Herein, we describe the introduction of metallic Cu nanoparticles (NPs) on Cu2O films to change the product distribution from gaseous products on bare Cu2O to predominantly CH3OH by CO2 reduction in aqueous solutions. The specifically designed Cu/Cu2O interfaces balance the binding strengths of H* and CO* intermediates, which play critical roles in CH3OH production. With a TiO2 model photoanode to construct a photoelectrochemical cell, a Cu/Cu2O dark cathode exhibited a Faradaic efficiency of up to 53.6 % for CH3OH production. This work demonstrates the feasibility and mechanism of interface engineering to enhance the CH3OH production from CO2 reduction in aqueous electrolytes. Metallic copper nanoparticles were deposited on Cu2O films to change the product distribution of CO2 reduction in aqueous solution from the gaseous products generated on bare Cu2O to predominantly methanol. The carefully designed Cu/Cu2O interfaces balance the binding strengths of the H* and CO* intermediates, which enables efficient methanol production. [ABSTRACT FROM AUTHOR]
- Published
- 2018
- Full Text
- View/download PDF
30. Low‐Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance.
- Author
-
Zhu, Wenjin, Zhang, Lei, Yang, Piaoping, Hu, Congling, Luo, Zhibin, Chang, Xiaoxia, Zhao, Zhi‐Jian, and Gong, Jinlong
- Subjects
THIN films ,PALLADIUM ,NANOSTRUCTURED materials ,CARBON dioxide ,ELECTROLYTIC reduction - Abstract
Abstract: Electrochemical conversion of carbon dioxide (CO
2 ) to value‐added products is a possible way to decrease the problems resulting from CO2 emission. Thanks to the eminent conductivity and proper adsorption to intermediates, Pd has become a promising candidate for CO2 electroreduction (CO2 ER). However, Pd‐based nanocatalysts generally need a large overpotential. Herein we describe that ultrathin Pd nanosheets effectively reduce the onset potential for CO by exposing abundant atoms with comparatively low generalized coordination number. Hexagonal Pd nanosheets with 5 atomic thickness and 5.1 nm edge length reached CO faradaic efficiency of 94 % at −0.5 V, without any decay after a stability test of 8 h. It appears to be the most efficient among all of Pd‐based catalysts toward CO2 ER. Uniform hexagonal morphology made it reasonable to build models and take DFT calculations. The enhanced activity originates from mainly edge sites on palladium nanosheets. [ABSTRACT FROM AUTHOR]- Published
- 2018
- Full Text
- View/download PDF
31. Surface, Bulk, and Interface: Rational Design of Hematite Architecture toward Efficient Photo‐Electrochemical Water Splitting.
- Author
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Li, Chengcheng, Luo, Zhibin, Wang, Tuo, and Gong, Jinlong
- Published
- 2018
- Full Text
- View/download PDF
32. The Functionality of Surface Hydroxy Groups on the Selectivity and Activity of Carbon Dioxide Reduction over Cuprous Oxide in Aqueous Solutions.
- Author
-
Yang, Piaoping, Zhao, Zhi‐Jian, Chang, Xiaoxia, Mu, Rentao, Zha, Shenjun, Zhang, Gong, and Gong, Jinlong
- Subjects
CARBON dioxide ,CUPROUS oxide ,CATALYSTS ,HYDROGEN evolution reactions ,DENSITY functional theory - Abstract
Abstract: Carbon dioxide (CO
2 ) reduction in aqueous solutions is an attractive strategy for carbon capture and utilization. Cuprous oxide (Cu2 O) is a promising catalyst for CO2 reduction as it can convert CO2 into valuable hydrocarbons and suppress the side hydrogen evolution reaction (HER). However, the nature of the active sites in Cu2 O remains under debate because of the complex surface structure of Cu2 O under reducing conditions, leading to limited guidance in designing improved Cu2 O catalysts. This paper describes the functionality of surface‐bonded hydroxy groups on partially reduced Cu2 O(111) for the CO2 reduction reaction (CO2 RR) by combined density functional theory (DFT) calculations and experimental studies. We find that the surface hydroxy groups play a crucial role in the CO2 RR and HER, and a moderate coverage of hydroxy groups is optimal for promotion of the CO2 RR and suppression of the HER simultaneously. Electronic structure analysis indicates that the charge transfer from hydroxy groups to coordination‐unsaturated Cu (CuCUS ) sites stabilizes surface‐adsorbed COOH*, which is a key intermediate during the CO2 RR. Moreover, the CO2 RR was evaluated over Cu2 O octahedral catalysts with {111} facets and different surface coverages of hydroxy groups, which demonstrates that Cu2 O octahedra with moderate coverage of hydroxy groups can indeed enhance the CO2 RR and suppress the HER. [ABSTRACT FROM AUTHOR]- Published
- 2018
- Full Text
- View/download PDF
33. Hydroxyl‐Mediated Non‐oxidative Propane Dehydrogenation over VOx/γ‐Al2O3 Catalysts with Improved Stability.
- Author
-
Zhao, Zhi‐Jian, Wu, Tengfang, Xiong, Chuanye, Sun, Guodong, Mu, Rentao, Zeng, Liang, and Gong, Jinlong
- Subjects
PROPANE ,DEHYDROGENATION ,VANADIUM catalysts ,CHEMICAL stability ,CHEMICAL reactions - Abstract
Abstract: Supported vanadium oxides are one of the most promising alternative catalysts for propane dehydrogenation (PDH) and efforts have been made to improve its catalytic performance. However, unlike Pt‐based catalysts, the nature of the active site and surface structure of the supported vanadium catalysts under reductive reaction conditions still remain elusive. This paper describes the surface structure and the important role of surface‐bound hydroxyl groups on VO
x / γ‐Al2 O3 catalysts under reaction conditions employing in situ DRIFTS experiments and DFT calculations. It is shown that hydroxyl groups on the VOx /Al2 O3 catalyst (V−OH) are produced under H2 pre‐reduction, and the catalytic performance for PDH is closely connected to the concentration of V−OH species on the catalyst. The hydroxyl groups are found to improve the catalyst that leads to better stability by suppressing the coke deposition. [ABSTRACT FROM AUTHOR]- Published
- 2018
- Full Text
- View/download PDF
34. Promoted Fixation of Molecular Nitrogen with Surface Oxygen Vacancies on Plasmon‐Enhanced TiO2 Photoelectrodes.
- Author
-
Li, Chengcheng, Wang, Tuo, Zhao, Zhi‐Jian, Yang, Weimin, Li, Jian‐Feng, Li, Ang, Yang, Zhilin, Ozin, Geoffrey A., and Gong, Jinlong
- Subjects
TITANIUM oxides ,HABER-Bosch process ,GREENHOUSE gases ,ADSORPTION (Chemistry) ,CLIMATE change ,CLEAN energy - Abstract
Abstract: A hundred years on, the energy‐intensive Haber–Bosch process continues to turn the N
2 in air into fertilizer, nourishing billions of people while causing pollution and greenhouse gas emissions. The urgency of mitigating climate change motivates society to progress toward a more sustainable method for fixing N2 that is based on clean energy. Surface oxygen vacancies (surface Ovac ) hold great potential for N2 adsorption and activation, but introducing Ovac on the very surface without affecting bulk properties remains a great challenge. Fine tuning of the surface Ovac by atomic layer deposition is described, forming a thin amorphous TiO2 layer on plasmon‐enhanced rutile TiO2 /Au nanorods. Surface Ovac in the outer amorphous TiO2 thin layer promote the adsorption and activation of N2 , which facilitates N2 reduction to ammonia by excited electrons from ultraviolet‐light‐driven TiO2 and visible‐light‐driven Au surface plasmons. The findings offer a new approach to N2 photofixation under ambient conditions (that is, room temperature and atmospheric pressure). [ABSTRACT FROM AUTHOR]- Published
- 2018
- Full Text
- View/download PDF
35. Synergism of Geometric Construction and Electronic Regulation: 3D Se‐(NiCo)S<italic>x</italic>/(OH)<italic>x</italic> Nanosheets for Highly Efficient Overall Water Splitting.
- Author
-
Hu, Congling, Zhang, Lei, Zhao, Zhi‐Jian, Li, Ang, Chang, Xiaoxia, and Gong, Jinlong
- Published
- 2018
- Full Text
- View/download PDF
36. Morphological and Compositional Design of Pd–Cu Bimetallic Nanocatalysts with Controllable Product Selectivity toward CO2 Electroreduction.
- Author
-
Zhu, Wenjin, Zhang, Lei, Yang, Piaoping, Chang, Xiaoxia, Dong, Hao, Li, Ang, Hu, Congling, Huang, Zhiqi, Zhao, Zhi‐Jian, and Gong, Jinlong
- Published
- 2018
- Full Text
- View/download PDF
37. Structure and catalytic consequence of Mg-modified VOx/Al2O3 catalysts for propane dehydrogenation.
- Author
-
Wu, Tengfang, Liu, Gang, Zeng, Liang, Sun, Guodong, Chen, Sai, Mu, Rentao, Agbotse Gbonfoun, Sika, Zhao, Zhi‐Jian, and Gong, Jinlong
- Subjects
VANADIUM oxide ,VANADIUM catalysts ,MAGNESIUM ,PROPANE ,DEHYDROGENATION - Abstract
Supported VO
x catalysts are promising nonoxidative propane dehydrogenation (PDH) materials for their commercially attractive activity and propylene selectivity. However, they frequently suffer from rapid deactivation caused by coke deposition. This article describes the promoting role of magnesium on the stability of VOx /Al2 O3 catalysts for PDH. A series of VOx /Al2 O3 and Mg-modified VOx /Al2 O3 catalysts were synthesized by an incipient wetness impregnation method. The catalysts were carefully characterized by Raman spectra, UV-Vis spectra, STEM, TGA and in situ DRIFTS. We showed that the stability of a 12V/Al2 O3 catalyst was significantly improved on addition of small amounts of MgO. Experimental evidences indicate that V2 O5 nanoparticles emerge in the 12V/Al2 O3 samples, and appropriate Mg addition helps dispersing the V2 O5 nanoparticles into 2D VOx species thus decreasing coke formation and improving stability in nonoxidative dehydrogenation of propane. © 2017 American Institute of Chemical Engineers AIChE J, 2017 [ABSTRACT FROM AUTHOR]- Published
- 2017
- Full Text
- View/download PDF
38. A Low-Cost NiO Hole Transfer Layer for Ohmic Back Contact to Cu2O for Photoelectrochemical Water Splitting.
- Author
-
Wei, Yijia, Chang, Xiaoxia, Wang, Tuo, Li, Chengcheng, and Gong, Jinlong
- Published
- 2017
- Full Text
- View/download PDF
39. Dendritic Hematite Nanoarray Photoanode Modified with a Conformal Titanium Dioxide Interlayer for Effective Charge Collection.
- Author
-
Luo, Zhibin, Wang, Tuo, Zhang, Jijie, Li, Chengcheng, Li, Huimin, and Gong, Jinlong
- Subjects
HEMATITE ,ANODES ,TITANIUM dioxide ,PASSIVATION ,DOPING agents (Chemistry) - Abstract
This paper describes the introduction of a thin titanium dioxide interlayer that serves as passivation layer and dopant source for hematite (α-Fe
2 O3 ) nanoarray photoanodes. This interlayer is demonstrated to boost the photocurrent by suppressing the substrate/hematite interfacial charge recombination, and to increase the electrical conductivity by enabling Ti4+ incorporation. The dendritic nanostructure of this photoanode with an increased solid-liquid junction area further improves the surface charge collection efficiency, generating a photocurrent of about 2.5 mA cm−2 at 1.23 V versus the reversible hydrogen electrode (vs. RHE) under air mass 1.5G illumination. A photocurrent of approximately 3.1 mA cm−2 at 1.23 V vs. RHE could be achieved by addition of an iron oxide hydroxide cocatalyst. [ABSTRACT FROM AUTHOR]- Published
- 2017
- Full Text
- View/download PDF
40. Edge Sites with Unsaturated Coordination on Core-Shell Mn3O4@Mn xCo3− xO4 Nanostructures for Electrocatalytic Water Oxidation.
- Author
-
Hu, Congling, Zhang, Lei, Zhao, Zhi‐Jian, Luo, Jun, Shi, Jing, Huang, Zhiqi, and Gong, Jinlong
- Published
- 2017
- Full Text
- View/download PDF
41. Nanostructured Materials for Heterogeneous Electrocatalytic CO2 Reduction and their Related Reaction Mechanisms.
- Author
-
Zhang, Lei, Zhao, Zhi‐Jian, and Gong, Jinlong
- Subjects
NANOSTRUCTURED materials ,HETEROGENEOUS catalysis ,ELECTROCATALYSIS ,CARBON dioxide reduction ,CHEMICAL reactions - Abstract
The gradually increased concentration of carbon dioxide (CO
2 ) in the atmosphere has been recognized as the primary culprit for the rise of the global mean temperature. In recent years, development of routes for highly efficient conversion of CO2 has received much attention. This Review describes recent progress on the design and synthesis of solid-state catalysts for the electrochemical reduction of CO2 . The significance of this catalytic conversion is presented, followed by the general parameters for CO2 electroreduction and a summary of the reaction apparatus. We also discuss various types of solid catalysts based on their CO2 conversion mechanisms. We summarize the crucial factors (particle size, surface structure, composition, etc.) determining the performance for electroreduction. [ABSTRACT FROM AUTHOR]- Published
- 2017
- Full Text
- View/download PDF
42. Nanostrukturierte Materialien für die elektrokatalytische CO2-Reduktion und ihre Reaktionsmechanismen.
- Author
-
Zhang, Lei, Zhao, Zhi‐Jian, and Gong, Jinlong
- Abstract
Copyright of Angewandte Chemie is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
- Published
- 2017
- Full Text
- View/download PDF
43. Facile synthesis of Pd@Pt octahedra supported on carbon for electrocatalytic applications.
- Author
-
Yu, Shengnan, Zhang, Lei, Dong, Hao, and Gong, Jinlong
- Subjects
PALLADIUM ,PLATINUM ,ELECTROCATALYSIS ,CRYSTAL morphology ,OXIDATION - Abstract
Due to the scarcity of Pt, it is highly desirable to construct core-shell structures with ultrathin Pt shells while maintaining their high electrocatalytic activities. However, it is necessary to preferentially synthesize a core with a specific structure before further formation of core-shell catalysts with specific morphologies. This prerequisite greatly increases the complexity of the synthesis process. This article describes a synthetic method of core-shell Pd@Pt octahedra catalysts from Pd nanocubes, truncated nanocubes or truncated octahedra. The formation of octahedral core-shell structures involves two key factors: (1) the oxidative etching process of Pd atoms at the corner sites; (2) the different reduction rates between Pt and Pd precursors. This mechanism can be extended to synthesize carbon-supported sub-8 nm Pd@Pt octahedra from commercial Pd/C catalysts. The derived carbon-supported Pd@Pt octahedra catalysts performed comparable activity and durability for methanol oxidation reaction with state-of-art PtRu/C catalysts. This synthetic method provides an innovative path for large-scale production of well-controlled catalysts. © 2017 American Institute of Chemical Engineers AIChE J, 63: 2528-2534, 2017 [ABSTRACT FROM AUTHOR]
- Published
- 2017
- Full Text
- View/download PDF
44. Surviving High-Temperature Calcination: ZrO2-Induced Hematite Nanotubes for Photoelectrochemical Water Oxidation.
- Author
-
Li, Chengcheng, Li, Ang, Luo, Zhibin, Zhang, Jijie, Chang, Xiaoxia, Huang, Zhiqi, Wang, Tuo, and Gong, Jinlong
- Subjects
CALCINATION (Heat treatment) ,ZIRCONIUM oxide ,IRON oxides ,HEMATITE ,PHOTOELECTROCHEMICAL cells ,PHOTOCURRENTS - Abstract
Nanotubular Fe
2 O3 is a promising photoanode material, and producing morphologies that withstand high-temperature calcination (HTC) is urgently needed to enhance the photoelectrochemical (PEC) performance. This work describes the design and fabrication of Fe2 O3 nanotube arrays that survive HTC for the first time. By introducing a ZrO2 shell on hydrothermal FeOOH nanorods by atomic layer deposition, subsequent high-temperature solid-state reaction converts FeOOH-ZrO2 nanorods to ZrO2 -induced Fe2 O3 nanotubes (Zr-Fe2 O3 NTs). The structural evolution of the hematite nanotubes is systematically explored. As a result of the nanostructuring and shortened charge collection distance, the nanotube photoanode shows a greatly improved PEC water oxidation activity, exhibiting a photocurrent density of 1.5 mA cm−2 at 1.23 V (vs. reversible hydrogen electrode, RHE), which is the highest among hematite nanotube photoanodes without co-catalysts. Furthermore, a Co-Pi decorated Zr-Fe2 O3 NT photoanode reveals an enhanced onset potential of 0.65 V (vs. RHE) and a photocurrent of 1.87 mA cm−2 (at 1.23 V vs. RHE). [ABSTRACT FROM AUTHOR]- Published
- 2017
- Full Text
- View/download PDF
45. Effects of Ga doping on Pt/CeO2-Al2O3 catalysts for propane dehydrogenation.
- Author
-
Wang, Tuo, Jiang, Feng, Liu, Gang, Zeng, Liang, Zhao, Zhi‐jian, and Gong, Jinlong
- Subjects
DEHYDROGENATION ,DENSITY functional theory ,CATALYSTS ,CHEMISORPTION ,DESORPTION - Abstract
This paper describes catalytic consequencesThis paper describes catalytic consequences of Pt/CeO
2 -Al2 O3 catalysts promoted with Ga species for propane dehydrogenation. A series of PtGa/CeO2 -Al2 O3 catalysts were prepared by a sequential impregnation method. The as-prepared catalysts were characterized employing N2 adsorption-desorption, X-ray diffrtaction, temperature programmed reduction, O2 volumetric chemisorption, H2 -O2 titration, and transmission electron microscopy. We have shown that Ga3+ cations are incorporated into the cubic fluorite structure of CeO2 , enhancing both lattice oxygen storage capacity and surface oxygen mobility. The enhanced reducibility of CeO2 is indicative of higher capability to eliminate the coke deposition and thus is beneficial to the improvement of catalytic stability. Density functional theory calculations confirm that the addition of Ga is prone to improve propylene desorption and greatly suppress deep dehydrogenation and the following coke formation. The catalytic performance shows a strong dependence on the content of Ga addition. The optimal loading content of Ga is 3 wt %, which results in the maximal propylene selectivity together with the best catalytic stability against coke accumulation. © 2016 American Institute of Chemical Engineers AIChE J, 62: 4365-4376, 2016 [ABSTRACT FROM AUTHOR]- Published
- 2016
- Full Text
- View/download PDF
46. Heterogeneous Molecular Systems for Photocatalytic CO2 Reduction with Water Oxidation.
- Author
-
Liu, Xiao, Inagaki, Shinji, and Gong, Jinlong
- Subjects
PHOTOSYNTHESIS ,OXIDATION ,QUANTUM chemistry ,QUANTUM efficiency ,PHOTOSYSTEMS ,CHLOROPHYLL-binding proteins - Abstract
Artificial photosynthesis-reduction of CO
2 into chemicals and fuels with water oxidation in the presence of sunlight as the energy source-mimics natural photosynthesis in green plants, and is considered to have a significant part to play in future energy supply and protection of our environment. The high quantum efficiency and easy manipulation of heterogeneous molecular photosystems based on metal complexes enables them to act as promising platforms to achieve efficient conversion of solar energy. This Review describes recent developments in the heterogenization of such photocatalysts. The latest state-of-the-art approaches to overcome the drawbacks of low durability and inconvenient practical application in homogeneous molecular systems are presented. The coupling of photocatalytic CO2 reduction with water oxidation through molecular devices to mimic natural photosynthesis is also discussed. [ABSTRACT FROM AUTHOR]- Published
- 2016
- Full Text
- View/download PDF
47. Heterogene molekulare Systeme für eine photokatalytische CO2-Reduktion mit Wasseroxidation.
- Author
-
Liu, Xiao, Inagaki, Shinji, and Gong, Jinlong
- Abstract
Copyright of Angewandte Chemie is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
- Published
- 2016
- Full Text
- View/download PDF
48. Thin Heterojunctions and Spatially Separated Cocatalysts To Simultaneously Reduce Bulk and Surface Recombination in Photocatalysts.
- Author
-
Li, Ang, Chang, Xiaoxia, Huang, Zhiqi, Li, Chengcheng, Wei, Yijia, Zhang, Lei, Wang, Tuo, and Gong, Jinlong
- Subjects
HETEROJUNCTIONS ,CATALYSTS ,BULK solids ,SURFACE recombination ,PHOTOCATALYSTS ,SEPARATION (Technology) - Abstract
Efficient charge separation and light absorption are crucial for solar energy conversion over solid photocatalysts. This paper describes the construction of Pt@TiO
2 @In2 O3 @MnOx mesoporous hollow spheres (PTIM-MSs) for highly efficient photocatalytic oxidation. TiO2 -In2 O3 double-layered shells were selectively decorated with Pt nanoparticles and MnOx on the inner and outer surfaces, respectively. The spatially separated cocatalysts drive electrons and holes near the surface to flow in opposite directions, while the thin heterogeneous shell separates the charges generated in the bulk phase. The synergy between the thin heterojunctions and the spatially separated cocatalysts can simultaneously reduce bulk and surface/subsurface recombination. In2 O3 also serves as a sensitizer to enhance light absorption. The PTIM-MSs exhibit high photocatalytic activity for both water and alcohol oxidation. [ABSTRACT FROM AUTHOR]- Published
- 2016
- Full Text
- View/download PDF
49. Stable Aqueous Photoelectrochemical CO2 Reduction by a Cu2O Dark Cathode with Improved Selectivity for Carbonaceous Products.
- Author
-
Chang, Xiaoxia, Wang, Tuo, Zhang, Peng, Wei, Yijia, Zhao, Jiubing, and Gong, Jinlong
- Subjects
CATHODES ,CARBONACEOUS aerosols ,PHOTOCATALYSIS ,ELECTROLYTES ,ELECTRONS - Abstract
Photocatalytic reduction of CO
2 to produce fuels is a promising way to reduce CO2 emission and address the energy crisis. However, the H2 evolution reaction competes with CO2 photoreduction, which would lower the overall selectivity for carbonaceous products. Cu2 O has emerged as a promising material for suppressing the H2 evolution. However, it suffers from poor stability, which is commonly regarded as the result of the electron-induced reduction of Cu2 O. This paper describes a simple strategy using Cu2 O as a dark cathode and TiO2 as a photoanode to achieve stable aqueous CO2 reduction with a high Faradaic efficiency of 87.4 % and a selectivity of 92.6 % for carbonaceous products. We have shown that the photogenerated holes, instead of the electrons, primarily account for the instability of Cu2 O. Therefore, Cu2 O was used as a dark cathode to minimize the adverse effects of holes, by which an improved stability was achieved compared to the Cu2 O photocathode under illumination. Additionally, direct exposure of the Cu2 O surface to the electrolyte was identified as a critical factor for the high selectivity for carbonaceous products. [ABSTRACT FROM AUTHOR]- Published
- 2016
- Full Text
- View/download PDF
50. Enhanced Charge Separation through ALD-Modified Fe2O3 /Fe2TiO5 Nanorod Heterojunction for Photoelectrochemical Water Oxidation.
- Author
-
Li, Chengcheng, Wang, Tuo, Luo, Zhibin, Liu, Shanshan, and Gong, Jinlong
- Published
- 2016
- Full Text
- View/download PDF
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