13 results on '"Liu, Shoujie"'
Search Results
2. The Heterointerface between Fe1/NC and Selenides Boosts Reversible Oxygen Electrocatalysis.
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Zheng, Huanran, Wang, Shibin, Liu, Shoujie, Wu, Jiao, Guan, Jianping, Li, Qian, Wang, Yuchao, Tao, Yu, Hu, Shouyao, Bai, Yu, Wang, Jinxian, Xiong, Xiang, Xiong, Yu, and Lei, Yongpeng
- Subjects
OXYGEN reduction ,ELECTROCATALYSIS ,OXYGEN evolution reactions ,CATALYTIC activity ,SELENIDES ,DENSITY functional theory ,CHARGE exchange - Abstract
The rational design and construction of efficient and inexpensive bifunctional oxygen electrocatalysts are highly desirable for the development of rechargeable Zn–air batteries (ZABs). Although single‐atom Fe sites anchored on N‐doped carbon catalysts (Fe1/NC) ensure high oxygen reduction reaction activity, their unitary atomically dispersed active center faces difficult condition in catalyzing oxygen evolution reaction simultaneously. Herein, a composite catalyst containing heterointerface between Fe1/NC and selenides ((Fe,Co)Se2) is constructed. The obtained (Fe,Co)Se2@Fe1/NC exhibits extremely narrow potential gap of 0.616 V and remarkable stability in alkaline media, outperforming the benchmark catalysts (Pt/C+RuO2: 0.720 V). Experimental results and density functional theory calculations reveal that heterointerface between Fe1/NC and (Fe,Co)Se2 accelerates the electron transfer and provides more moderate adsorption sites, which endow (Fe,Co)Se2@Fe1/NC with extremely high bifunctional oxygen catalytic activity. This study not only provides a superior bifunctional catalyst for ZABs, but also enriches the application of single‐atom catalysts in multifunctional energy storage and conversion devices. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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3. In Situ Periodic Regeneration of Catalyst during CO2 Electroreduction to C2+ Products.
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Xu, Liang, Ma, Xiaodong, Wu, Limin, Tan, Xingxing, Song, Xinning, Zhu, Qinggong, Chen, Chunjun, Qian, Qingli, Liu, Zhimin, Sun, Xiaofu, Liu, Shoujie, and Han, Buxing
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COUPLING reactions (Chemistry) ,CATALYSTS ,CARBON offsetting ,ELECTROLYTIC reduction ,SURFACE structure ,OXIDATION states ,CATALYTIC cracking - Abstract
Developing electrocatalytic reactions with high‐efficiency can make important contributions to carbon neutrality. However, poor long‐term stability of catalysts is a bottleneck for its practical application. Herein, an "in situ periodic regeneration of catalyst (PR‐C)" strategy is proposed to give long‐term high efficiency of CO2 electroreduction to generate C2+ products over Cu catalyst by applying a positive potential pulse for a short time periodically in the halide‐containing electrolyte. The high Faradaic efficiency (81.2 %) and current density (22.6 mA cm−2) could be maintained completely at least 36 h, while the activity and selectivity decreased continuously without using the PR‐C method. Control experiments and operando characterization demonstrated that the surface structure and oxidation state of Cu could be recovered periodically by the PR‐C method, which was beneficial for CO2 activation and C−C coupling. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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4. Boosting the Productivity of Electrochemical CO2 Reduction to Multi‐Carbon Products by Enhancing CO2 Diffusion through a Porous Organic Cage.
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Chen, Chunjun, Yan, Xupeng, Wu, Yahui, Liu, Shoujie, Zhang, Xiudong, Sun, Xiaofu, Zhu, Qinggong, Wu, Haihong, and Han, Buxing
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SURFACE diffusion ,CARBON dioxide ,ELECTROLYTIC reduction - Abstract
Electroreduction of CO2 into valuable fuels and feedstocks offers a promising way for CO2 utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO2 electroreduction by improving diffusion of CO2 to the surface of catalysts using porous organic cages (POCs) as an additive. It was noted that the Faradaic efficiency (FE) of C2+ products could reach 76.1 % with a current density of 1.7 A cm−2 when Cu‐nanorod(nr)/CC3 (one of the POCs) was used, which were much higher than that using Cu‐nr. Detailed studies demonstrated that the hydrophobic pores of CC3 can adsorb a large amount of CO2 for the reaction, and the diffusion of CO2 in the CC3 to the nanocatalyst surface is easier than that in the liquid electrolyte. Thus, more CO2 molecules make contact with the nanocatalysts in the presence of CC3, enhancing CO2 reduction and inhibiting generation of H2. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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5. Highly Efficient CO2 Electroreduction to Methanol through Atomically Dispersed Sn Coupled with Defective CuO Catalysts.
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Guo, Weiwei, Liu, Shoujie, Tan, Xingxing, Wu, Ruizhi, Yan, Xupeng, Chen, Chunjun, Zhu, Qinggong, Zheng, Lirong, Ma, Jingyuan, Zhang, Jing, Huang, Yuying, Sun, Xiaofu, and Han, Buxing
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CATALYSTS , *TIN , *ELECTROLYTIC reduction , *METHANOL , *ACTIVATION energy , *DENSITY functional theory - Abstract
Using renewable electricity to drive CO2 electroreduction is an attractive way to achieve carbon‐neutral energy cycle and produce value‐added chemicals and fuels. As an important platform molecule and clean fuel, methanol requires 6‐electron transfer in the process of CO2 reduction. Currently, CO2 electroreduction to methanol suffers from poor efficiency and low selectivity. Herein, we report the first work to design atomically dispersed Sn site anchored on defective CuO catalysts for CO2 electroreduction to methanol. It exhibits high methanol Faradaic efficiency (FE) of 88.6 % with a current density of 67.0 mA cm−2 and remarkable stability in a H‐cell, which is the highest FE(methanol) with such high current density compared with the results reported to date. The atomic Sn site, adjacent oxygen vacancy and CuO support cooperate very well, leading to higher double‐layer capacitance, larger CO2 adsorption capacity and lower interfacial charge transfer resistance. Operando experiments and density functional theory calculations demonstrate that the catalyst is beneficial for CO2 activation via decreasing the energy barrier of *COOH dissociation to form *CO. The obtained key intermediate *CO is then bound to the Cu species for further reduction, leading to high selectivity toward methanol. [ABSTRACT FROM AUTHOR]
- Published
- 2021
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6. Boosting CO2 Electroreduction over a Cadmium Single‐Atom Catalyst by Tuning of the Axial Coordination Structure.
- Author
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Wu, Yahui, Chen, Chunjun, Yan, Xupeng, Sun, Xiaofu, Zhu, Qinggong, Li, Pengsong, Li, Yiming, Liu, Shoujie, Ma, Jingyuan, Huang, Yuying, and Han, Buxing
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HYDROGEN evolution reactions ,ELECTROLYTIC reduction ,CATALYSTS ,ACTIVATION energy ,CADMIUM ,COORDINATION polymers ,ELECTROLYSIS - Abstract
Guided by first‐principles calculations, it was found that Cd single‐atom catalysts (SACs) have excellent performance in activating CO2, and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO2 reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN4S1 moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO2 electroreduction to CO. The faradaic efficiency (FE) of CO could reach up to 99.7 % with a current density of 182.2 mA cm−2 in a H‐type electrolysis cell, and the turnover frequency (TOF) value could achieve 73000 h−1, which was much higher than that reported to date. This work shows a successful example of how to design highly efficient catalysts guided by theoretical calculations. [ABSTRACT FROM AUTHOR]
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- 2021
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7. Highly Efficient Electroreduction of CO2 to C2+ Alcohols on Heterogeneous Dual Active Sites.
- Author
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Chen, Chunjun, Yan, Xupeng, Liu, Shoujie, Wu, Yahui, Wan, Qiang, Sun, Xiaofu, Zhu, Qinggong, Liu, Huizhen, Ma, Jun, Zheng, Lirong, Wu, Haihong, and Han, Buxing
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ELECTROLYTIC reduction ,ETHANOL as fuel ,LIQUID fuels ,ALCOHOL ,QUANTUM dots ,PROPANOLS - Abstract
Electroreduction of CO2 to liquid fuels such as ethanol and n‐propanol, powered by renewable electricity, offers a promising strategy for controlling the global carbon balance and addressing the need for the storage of intermittent renewable energy. In this work, we discovered that the composite composed of nitrogen‐doped graphene quantum dots (NGQ) on CuO‐derived Cu nanorods (NGQ/Cu‐nr) was an outstanding electrocatalyst for the reduction of CO2 to ethanol and n‐propanol. The Faradaic efficiency (FE) of C2+ alcohols could reach 52.4 % with a total current density of 282.1 mA cm−2. This is the highest FE for C2+ alcohols with a commercial current density to date. Control experiments and DFT studies show that the NGQ/Cu‐nr could provide dual catalytic active sites and could stabilize the CH2CHO intermediate to enhance the FE of alcohols significantly through further carbon protonation. The NGQ and Cu‐nr had excellent synergistic effects for accelerating the reduction of CO2 to alcohols. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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8. Synergistically Interactive Pyridinic‐N–MoP Sites: Identified Active Centers for Enhanced Hydrogen Evolution in Alkaline Solution.
- Author
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Zhao, Di, Sun, Kaian, Cheong, Weng‐Chon, Zheng, Lirong, Zhang, Chao, Liu, Shoujie, Cao, Xing, Wu, Konglin, Pan, Yuan, Zhuang, Zewen, Hu, Botao, Wang, Dingsheng, Peng, Qing, Chen, Chen, and Li, Yadong
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ALKALINE solutions ,HYDROGEN evolution reactions ,OXYGEN reduction ,NANOPARTICLES ,TRANSITION metals ,HYDROGEN ,PHOSPHIDES - Abstract
For electrocatalysts for the hydrogen evolution reaction (HER), encapsulating transition metal phosphides (TMPs) into nitrogen‐doped carbon materials has been known as an effective strategy to elevate the activity and stability. Yet still, it remains unclear how the TMPs work synergistically with the N‐doped support, and which N configuration (pyridinic N, pyrrolic N, or graphitic N) contributes predominantly to the synergy. Here we present a HER electrocatalyst (denoted as MoP@NCHSs) comprising MoP nanoparticles encapsulated in N‐doped carbon hollow spheres, which displays excellent activity and stability for HER in alkaline media. Results of experimental investigations and theoretical calculations indicate that the synergy between MoP and the pyridinic N can most effectively promote the HER in alkaline media. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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9. Aqueous CO2 Reduction with High Efficiency Using α‐Co(OH)2‐Supported Atomic Ir Electrocatalysts.
- Author
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Sun, Xiaofu, Chen, Chunjun, Liu, Shoujie, Hong, Song, Zhu, Qinggong, Qian, Qingli, Han, Buxing, Zhang, Jing, and Zheng, Lirong
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ELECTROCATALYSTS ,CATALYTIC activity ,RADICAL anions ,CHARGE exchange ,ELECTROLYTIC reduction ,AQUEOUS electrolytes - Abstract
Electrochemical reduction of CO2 into energy‐dense chemical feedstock and fuels provides an attractive pathway to sustainable energy storage and artificial carbon cycle. Herein, we report the first work to use atomic Ir electrocatalyst for CO2 reduction. By using α‐Co(OH)2 as the support, the faradaic efficiency of CO could reach 97.6 % with a turnover frequency (TOF) of 38290 h−1 in aqueous electrolyte, which is the highest TOF up to date. The electrochemical active area is 23.4‐times higher than Ir nanoparticles (2 nm), which is highly conductive and favors electron transfer from CO2 to its radical anion (CO2.−). Moreover, the more efficient stabilization of CO2.− intermediate and easy charge transfer makes the atomic Ir electrocatalyst facilitate CO production. Hence, α‐Co(OH)2‐supported atomic Ir electrocatalysts show enhanced CO2 activity and stability. High‐density atomic Ir supported on α‐Co(OH)2 had outstanding performance for CO2 reduction to CO. The faradaic efficiency can reach 97.6 % with a TOF of 38 290 h−1. The high catalytic activity is attributed to more active sites for CO2 adsorption and activation and the higher efficiency in stabilizing the CO2.− intermediate. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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10. Porphyrin-like Fe-N4 sites with sulfur adjustment on hierarchical porous carbon for different rate-determining steps in oxygen reduction reaction.
- Author
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Wu, Konglin, Chen, Xin, Liu, Shoujie, Pan, Yuan, Cheong, Weng-Chon, Zhu, Wei, Cao, Xing, Shen, Rongan, Chen, Wenxing, Luo, Jun, Yan, Wensheng, Zheng, Lirong, Chen, Zheng, Wang, Dingsheng, Peng, Qing, Chen, Chen, and Li, Yadong
- Abstract
We developed a strategy based on coordination polymer to synthesize singleatom site Fe/N and S-codoped hierarchical porous carbon (Fe
1 /N,S-PC). The as-obtained Fe1 /N,S-PC exhibited superior oxygen reduction reaction (ORR) performance with a half-wave potential (E1/2 , 0.904 V vs. RHE) that was better than that of commercial Pt/C (E1/2 , 0.86 V vs. RHE), single-atom site Fe/N-doped hierarchical porous carbon (Fe1 /N-PC) without S-doped (E1/2 , 0.85 V vs. RHE), and many other nonprecious metal catalysts in alkaline medium. Moreover, the Fe1 /N,S-PC revealed high methanol tolerance and firm stability. The excellent electrocatalytic activity of Fe1 /N,S-PC is attributed to the synergistic effects from the atomically dispersed porphyrin-like Fe-N4 active sites, the heteroatom codoping (N and S), and the hierarchical porous structure in the carbon materials. The calculation based on density functional theory further indicates that the catalytic performance of Fe1 /N,S-PC is better than that of Fe1 /N-PC owing to the sulfur doping that yielded different rate-determining steps. [ABSTRACT FROM AUTHOR]- Published
- 2018
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11. Construction of CoP/NiCoP Nanotadpoles Heterojunction Interface for Wide pH Hydrogen Evolution Electrocatalysis and Supercapacitor.
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Lin, Yan, Sun, Kaian, Liu, Shoujie, Chen, Xiaomeng, Cheng, Yuansheng, Cheong, Weng‐Chon, Chen, Zheng, Zheng, Lirong, Zhang, Jun, Li, Xiyou, Pan, Yuan, and Chen, Chen
- Subjects
ELECTROCATALYSIS ,SOLID-state phase transformations ,HETEROJUNCTIONS ,HYDROGEN evolution reactions ,SURFACE energy ,ENERGY density - Abstract
Constructing well defined nanostructures is promising but still challenging for high‐efficiency catalysts for hydrogen evolution reaction (HER) and energy storage. Herein, utilizing the differences in surface energies between (111) facets of CoP and NiCoP, a novel CoP/NiCoP heterojunction is designed and synthesized with a nanotadpoles (NTs)‐like morphology via a solid‐state phase transformation strategy. By effective interface construction, the disorder in terms of electronic structure and coordination environment at the interface in CoP/NiCoP NTs is created, which leads to dramatically elevated HER performance within a wide pH range. Theoretical calculations prove that an optimized proton chemisorption and H2O dissociation are achieved by an optimized phosphide polymorph at the interface, accelerating the HER reaction. The CoP/NiCoP NTs are also proved to be excellent candidates for use in supercapacitors (SCs) with a high specific capacitance (1106.2 F g−1 at 1 A g−1) and good cycling stability (nearly 100% initial capacity retention after 1000 cycles). An asymmetric supercapacitor shows a high energy density (145 F g−1 at 1 A g−1) and good cycling stability (capacitance retention is 95% after 3200 cycles). This work provides new insights into the catalyst design for electrocatalytic and energy storage applications. [ABSTRACT FROM AUTHOR]
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- 2019
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12. Efficient electrocatalytic water splitting by bimetallic cobalt iron boride nanoparticles with controlled electronic structure.
- Author
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Qiang, Chenchen, Zhang, Liang, He, Hengli, Liu, Yangyang, Zhao, Yueying, Sheng, Tian, Liu, Shoujie, Wu, Xilin, and Fang, Zhen
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ELECTRONIC structure , *HYDROGEN evolution reactions , *OXYGEN evolution reactions , *X-ray photoelectron spectroscopy , *IRON catalysts , *COBALT , *CLEAN energy - Abstract
[Display omitted] • Bimetallic cobalt iron boride nanoparticle catalyst was successfully synthesized. • The bimetallic cobalt iron boride catalyst shows excellent over all water splitting performance. • Outstanding performance of the catalyst roots form the synergistic effect of the optimized electronic and composition. Developing an efficient bifunctional catalyst for Hydrogen Evolution Reaction (HER) and Oxygen Evolution Reaction (OER) in water splitting technology is very attractive for clean energy. Here, a new Co-Fe-B ternary catalyst with improved crystallinity is successfully synthesized by combining the chemical reduction and subsequent solid-state reaction method. Synchrotron-based X-ray absorption near-edge structure (XANES) and X-ray photoelectron spectroscopy (XPS) indicate the electronic structure redistribution is favor for the improved performance. The overpotential is only 129 mV and 280 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline condition, the corresponding Tafel slope is 67.3 mV dec−1 and 38.9 mV dec−1. Density functional theory calculations distinguish that the ternary crystalline Co-Fe-B catalysts are thermodynamically favorable for HER and OER. The actual active species of the ternary catalyst in OER is the CoOOH and FeOOH as indicated in ex situ Raman spectra. The present work may introduce promising crystallinity borides material for the anode and cathode of water splitting device. [ABSTRACT FROM AUTHOR]
- Published
- 2021
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13. Atomically dispersed Ni on Mo2C embedded in N, P co-doped carbon derived from polyoxometalate supramolecule for high-efficiency hydrogen evolution electrocatalysis.
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Lu, Yukun, Yue, Changle, Li, Yaping, Bao, Wenjing, Guo, Xinxin, Yang, Wenfeng, Liu, Zhi, Jiang, Ping, Yan, Wenfu, Liu, Shoujie, Pan, Yuan, and Liu, Yunqi
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ELECTROCATALYSIS , *HYDROGEN evolution reactions , *PHOSPHORUS , *HYDROGEN , *ATOMIC structure , *CATALYTIC activity , *CLEAN energy , *ENERGY conversion - Abstract
[Display omitted] • A supramolecular-confinement pyrolysis strategy is proposed to fabricate ultra-dispersed Ni-Mo 2 C nanoparticles. • POMs-based supramolecular aggregate act as pre-assembling molecular platform for regulating Mo 2 C structure at atomic level. • Atomically dispersed Ni doping and Ni-P catalyst-substrate coupling synergistically enhance the intrinsic activity of Mo 2 C. • Ni-Mo 2 C/NPC exhibits excellent electrocatalytic activity and durability for HER in acidic and alkaline conditions. • The EXAFS and DFT calculations confirm that Mo(C)–Ni–P configuration is the origin of outstanding HER activities. Herein, a novel supramolecular-confinement pyrolysis strategy was proposed to construct ultrafine Ni-Mo 2 C nanoparticles uniformly distributed on N,P co-doped carbon (NPC) by using polyoxometalate supramolecular aggregate as precursor. Ni-Mo 2 C/NPC exhibits remarkable electrocatalytic activity for hydrogen evolution reaction (HER) in both acidic and alkaline conditions, as well as superior long-term durability. Combining EXAFS with DFT calculations, we demonstrate that Ni species were atomically dispersed and anchored by Mo 2 C lattice and P atoms from NPC, thus defining Mo(C)–Ni–P active sites, which enhance the intrinsic catalytic activity of Mo 2 C by atomic-scale Ni doping and Ni–P catalyst-substrate chemical coupling. The Mo(C)–Ni–P sites have optimal hydrogen adsorption free energies and can precisely regulate and activate the neighboring C, leading to excellent HER performance. This work developed a "bottom-up" polyoxometalate-based supramolecular approach for in-situ assembly of high-active HER catalytic sites, which will provide opportunities to design and fabricate low-cost and efficient atomic-scale catalysts for clean energy conversion. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
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