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330 results on '"Chu, Shengqi"'

55. High-Entropy Anti-Perovskites with Negative Thermal Expansion Behavior

Author

Yuan, Xiuliang, Wang, Bing, Sun, Ying, Guo, Huaiming, Shi, Kewen, Deng, Sihao, He, Lunhua, Lu, Huiqing, Zhang, Hong, Xu, Shengdi, Du, Yi, Chu, Shengqi, Hao, Weichang, and Wang, Cong

Subjects
Condensed Matter - Materials Science, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences
Abstract

The negative thermal expansion (NTE) material is counterintuitive due to its typical feature of volume contraction on heating, which can act as the thermal-expansion compensators to counteract the normal positive thermal expansion. A wide temperature range of NTE behavior is desired, whereas the performance optimization by traditional doping strategy has reached its upper limit. In this paper, the unique sluggish characteristic in high entropy materials is proposed to broaden the NTE temperature range by relaxing the sharp phase transition in Mn-based anti-perovskite nitride. We propose an empirical screening method to synthesis the high-entropy anti-perovskite (HEAP). A remarkable NTE behavior (up to {\Delta}T = 235 K, 5 K < T < 240 K) with the coefficient of thermal expansion (CTE) of - 4.7 ppm/K has been observed in typical HEAP Mn3Cu0.2Zn0.2Ga0.2Ge0.2Mn0.2N, whose working temperature range is far wider than that of traditional low-entropy doping system. The wide temperature range of phase separation due to sluggish phase transition is responsible for the broadened NTE behavior in HEAP. Our demonstration provides a unique paradigm in the broadening of the NTE temperature range for phase transition induced NTE materials through entropy engineering., Comment: 22 pages, 5 figures

Published
2023
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62. Decreasing the Overpotential of Aprotic Li‐CO2 Batteries with the In‐Plane Alloy Structure in Ultrathin 2D Ru‐Based Nanosheets

Author

Wang, Yunhao, primary, Zhou, Jingwen, additional, Lin, Chao, additional, Chen, Bo, additional, Guan, Zhiqiang, additional, Ebrahim, Amani M., additional, Qian, Guannan, additional, Ye, Chenliang, additional, Chen, Lin, additional, Ge, Yiyao, additional, Yun, Qinbai, additional, Wang, Xixi, additional, Zhou, Xichen, additional, Wang, Gang, additional, Li, Kedi, additional, Lu, Pengyi, additional, Ma, Yangbo, additional, Xiong, Yuecheng, additional, Wang, Tianshuai, additional, Zheng, Long, additional, Chu, Shengqi, additional, Chen, Ye, additional, Wang, Bin, additional, Lee, Chun‐Sing, additional, Liu, Yijin, additional, Zhang, Qianfan, additional, and Fan, Zhanxi, additional

Published
2022
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63. Rb4Li2TiOGe4O12: a novel high-performance titanyl germanate anode for Li-ion batteries.

Author

Tang, Chuan, Chang, Siliang, Wu, Qian, Kang, Lei, Feng, Kai, Meng, Xianghe, Chu, Shengqi, Huang, Hongwei, and Xia, Mingjun

Abstract

The design of high-performance anode materials is the key to improving the performance of lithium-ion batteries. Here, a new high-performance titanyl germanate anode, Rb4Li2TiOGe4O12 (RLTG), was investigated for lithium-ion storage properties for the first time. Thanks to the multi-electron reactions of Ti and Ge and the polyanion framework, RLTG exhibits a high discharge specific capacity of 786.2 mA h g−1 and decent capacity retention performance of 84%. In addition, RLTG shows a good rate capability in the range of 0.05–2.5 A g−1. Furthermore, the discharge/charge behaviors were explored in depth by a cyclic voltammetry test, galvanostatic intermittent titration technique, X-ray absorption near-edge spectroscopy and electrochemical impedance spectroscopy, combined with first-principles calculations. [ABSTRACT FROM AUTHOR]

Published
2023
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69. Selective Oxidation of Methane into Formic Acid over ZIF‐8‐Encapsulated Mononuclear Fe Species under Mild Conditions.

Author

Lin, Lu, Zhang, Guikai, Kang, Liqun, Yu, Tao, Su, Yang, Zeng, Guang, Chu, Shengqi, and Luo, Wenhao

Subjects
OXIDATION of formic acid, FORMIC acid, MOSSBAUER spectroscopy, X-ray photoelectron spectroscopy, CATALYTIC oxidation, REFLECTANCE spectroscopy, ULTRAVIOLET spectroscopy, OXIDATION
Abstract

The direct catalytic oxidation of methane into C1 oxygenates is a promising approach for methane valorization. However, the difficulties in CH4 activation and inhibition of over‐oxidation hinder the development of efficient catalysts for this transformation. Herein, highly dispersed Fe species confined by ZIF‐8 are developed for the direct transformation of methane into value‐added C1 oxygenates with H2O2 as oxidant at 323 K. The as‐obtained Fe‐ZIF‐8 can afford an optimal turnover rate (TOR) of ∼45 molC1 molFe−1 h−1. Note that the selectivity to HCOOH is ∼97 %, outstanding among the reported Fe‐based heterogeneous catalysts. Combined analysis of X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, ultraviolet‐visible diffuse reflectance spectroscopy and 57Fe Mössbauer spectroscopy suggests that the catalytically active sites in Fe‐ZIF‐8 are mononuclear six‐coordinated Fe3+ species. The confinement of mononuclear Fe species within a porous metal‐organic framework material can provide an exquisite, enzyme‐like performance for highly selective oxidation of methane towards formic acid under mild conditions. [ABSTRACT FROM AUTHOR]

Published
2023
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70. Highly Selective Oxidation of Methane into Methanol over Cu-Promoted Monomeric Fe/ZSM-5

Author

Yu, Tao, Li, Zhi, Lin, Lu, Chu, Shengqi, Su, Yang, Song, Weiyu, Wang, Aiqin, Weckhuysen, Bert M., Luo, Wenhao, Inorganic Chemistry and Catalysis, and Sub Inorganic Chemistry and Catalysis

Subjects
Chemistry(all), copper, methane, monomeric Fe species, characterization, zeolite, Catalysis
Abstract

The selective oxidation of methane into methanol is of paramount importance but poses significant challenges in achieving high methanol productivity and selectivity, especially under mild reaction conditions. We show that a Cu-modified monomeric Fe/ZSM-5 catalyst is a highly efficient material for the direct conversion of methane into methanol in the liquid phase using H2O2 as an oxidant at low temperatures, which exhibits an excellent methanol productivity of 431 molMeOH·mol-1Fe·h-1 (with a methanol selectivity of μ80% over the Cu-Fe(2/0.1)/ZSM-5 catalyst). Combining the control experiments and comprehensive characterization results by among others, Mössbauer spectroscopy, and electron paramagnetic resonance as well as density functional theory calculations, we found that Cu species in the Cu-Fe(2/0.1)/ZSM-5 catalyst play a pivotal role in facilitating the formation of •OH radicals, which quickly react with •CH3 radicals to form CH3OH. These findings provide valuable insights into the rational design of metal-zeolite combinations for the selective oxidation of methane into methanol.

Published
2021

74. Highly Selective Oxidation of Methane into Methanol over Cu-Promoted Monomeric Fe/ZSM-5

Author

Inorganic Chemistry and Catalysis, Sub Inorganic Chemistry and Catalysis, Yu, Tao, Li, Zhi, Lin, Lu, Chu, Shengqi, Su, Yang, Song, Weiyu, Wang, Aiqin, Weckhuysen, Bert M., Luo, Wenhao, Inorganic Chemistry and Catalysis, Sub Inorganic Chemistry and Catalysis, Yu, Tao, Li, Zhi, Lin, Lu, Chu, Shengqi, Su, Yang, Song, Weiyu, Wang, Aiqin, Weckhuysen, Bert M., and Luo, Wenhao

Published
2021

79. Bifunctional CO oxidation over Mn-mullite anchored Pt sub-nanoclusters via atomic layer deposition† †Electronic supplementary information (ESI) available: Catalyst preparation and characterization details, supplemental figures and tables. See DOI: 10.1039/c7sc05486f

Author

Liu, Xiao, Tang, Yuanting, Shen, Meiqing, Li, Wei, Chu, Shengqi, Shan, Bin, and Chen, Rong

Subjects
Chemistry
Abstract

Highly dispersed Pt sub-nanoclusters are anchored on SmMn2O5 mullites via atomic layer deposition, and show excellent low-temperature CO oxidation activity., CO oxidation is a widely used model system for understanding fundamental aspects of heterogeneous catalysis. While platinum (Pt) continues to be a reference material for CO oxidation catalysis, poisoning of Pt catalysts presents a critical issue that blocks reaction sites and impedes subsequent reaction steps. Fabrication of CO poison-free Pt catalysts remains a great challenge due to its CO-philic nature. Herein, we report a Pt based catalyst to effectively tackle CO poisoning by tightly anchoring Pt sub-nanoclusters onto Mn-mullite oxide (SmMn2O5) via atomic layer deposition. Superior CO oxidation activity has been observed with a significantly lowered light-off temperature and apparent activation energy. In situ diffuse reflectance infrared Fourier transform spectroscopy analysis, oxygen isotope experiments and density functional theory calculations confirm that the low-temperature activity originates from active oxygen atom sources at the bifunctional interface structure.

Published
2018

80. Operando X-ray spectroscopy visualizing the chameleon-like structural reconstruction on an oxygen evolution electrocatalyst

Author

Cao, Dengfeng, primary, Liu, Daobin, additional, Chen, Shuangming, additional, Moses, Oyawale Adetunji, additional, Chen, Xingjia, additional, Xu, Wenjie, additional, Wu, Chuanqiang, additional, Zheng, Lirong, additional, Chu, Shengqi, additional, Jiang, Hongliang, additional, Wang, Changda, additional, Ge, Binghui, additional, Wu, Xiaojun, additional, Zhang, Jing, additional, and Song, Li, additional

Published
2021
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87. Surface Ligand Tuning of Coordination Geometry and Pb 6s2Electronic Pair Stereochemical Activity in MAPbBr3Perovskite Nanoparticles: A Joint Experimental and Theoretical Insight

Author

Yin, Zi, Liao, Jiangwen, Zhang, Guikai, Zuo, Shouwei, Chu, Shengqi, Zheng, Lirong, An, Pengfei, Huang, Huan, Dong, Juncai, and Zhang, Jing

Abstract

Surface ligand passivation strategies have been extensively used to produce metal halide perovskite nanoparticles (NPs) with excellent optoelectronic properties, and a better understanding of the ligand–NP interactions is essential to unleash the full potential of perovskite NPs. Here, the well-passivated methyl ammonium lead bromide NPs were obtained when (3-aminopropyl) triethoxysilane (APTES) and oleic acid (OA) were involved as efficient dual surface ligands. We systematically explored ligand–NP interactions by using spectroscopic analysis and theory calculations. Our results demonstrated that –[−OOC–R]−from OA would preferably occupy the Br vacancies on the surface under-coordinated Pb sites in the corner-sharing octahedral framework to form [PbBr5]3–-[−OOC–R]−complexes, whereas –NH3+of APTES can connect with Br–on the NP surface via hydrogen bonds. These surface binding interactions can trigger the lattice contraction of NPs, which can lead to an increased Pb2+off-centering by promoting the lone pair stereochemical activity. Furthermore, the electronic band structure can be modulated by orbital interactions within the inorganic Pb–Br frame through the surface ligand effect. This work not only increases our understanding of ligand–NP interactions in terms of coordination geometry but also reveals their influence on the stereochemical activity of the Pb 6s2electron pair, which will provide valuable inspiration for the ligand passivation strategies in the future.

Published
2022
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88. Application of X‐Ray Absorption Spectroscopy in Electrocatalytic Water Splitting and CO2 Reduction.

Author

Wang, Bin, Chu, Shengqi, Zheng, Lirong, Li, Xiaodong, Zhang, Jiangwei, and Zhang, Fuxiang

Abstract

Renewable energy conversion and storage are crucial in aiding the worldwide efforts to replace fossil fuels and achieve carbon neutrality. In particular, electrocatalytic water splitting to obtain H2 and CO2 reduction to high‐value‐added fuels can lead to an epoch of hydrogen energy and a closed‐loop carbon cycle. Although many reported electrocatalysts have demonstrated outstanding performance at the laboratory scale, the origin of the superior electrocatalytic activity and selectivity and the structural evolution of these catalysts remain ambiguous. For this purpose, operando techniques are able to combine the characterizations of the catalyst with measurement of its performance under real working conditions. Herein, a critical overview of recent developments in understanding the underlying mechanisms of water splitting and CO2 reduction is presented, emphasizing the advanced operando X‐ray absorption spectroscopy characterization of these two electrocatalytic reactions. Some perceptions of the rising X‐ray technique directions and the foreground in this field are also presented. [ABSTRACT FROM AUTHOR]

Published
2021
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93. Fabrication of a Single-Atom Platinum Catalyst for the Hydrogen Evolution Reaction: A New Protocol by Utilization of HxMoO3-xwith Plasmon Resonance

Author

Liu, Wei, Xu, Qun, Yan, Pengfei, Chen, Jun, Du, Yi, Chu, Shengqi, Wang, Jiaou, Liu, Wei, Xu, Qun, Yan, Pengfei, Chen, Jun, Du, Yi, Chu, Shengqi, and Wang, Jiaou

Abstract

Single-atom catalysts (SACs) play a key role in many chemical processes owing to highly desirable atom efficiency, but the challenging synthesis of these catalysts limits their commercialization and application on a large scale. Herein, we report a facile strategy to integrate atomic Pt into richly deficient MoO 3-x . The core of the experimental strategy was the fabrication and utilization of H x MoO 3-x with plasmon resonance that contained intercalated H + . The obtained catalyst was found to possess remarkable electrocatalytic activity toward the hydrogen evolution reaction that was even comparable to that of commercial Pt/C, whereas the amount of Pt used was reduced to only 10% of the amount of commercial Pt/C used. Therefore, this work not only supplies a new synthesis route to SACs but also reveals the potential relation between plasmon resonance materials and the fabrication of single-atom catalysts.

Published
2018

96. Highly dispersed Pt studded on CoOx nanoclusters for CO preferential oxidation in H2.

Author

Cai, Jiaming, Liu, Zhang, Cao, Kun, Lang, Yun, Chu, Shengqi, Shan, Bin, and Chen, Rong

Abstract

Carbon monoxide (CO) preferential oxidation (PROX) is regarded as a promising method for hydrogen purification. Herein, the design and synthesis of highly dispersed Pt studded on CoOx catalysts are reported. The catalysts exhibit nearly 100% CO conversion and selectivity towards the CO PROX reaction under H2 stream at room temperature. The superior catalytic performance can be attributed to the unique structure. The Pt is selectively studded on CoOx nanoclusters to maximize the highly active metal–oxide interfaces. The Pt loading is reduced to ∼0.8%, which is one of the lowest reported loadings for Pt-based CO PROX catalysts. The kinetics studies reveal that the composite Pt–Co catalysts have a weaker CO adsorption and lower O2 activation barrier, which can increase the CO oxidation rate and suppress the H2 oxidation rate. In addition, it is found that the CoOx promotor in a lower chemical oxidation state is critical for the improved activity. Theoretical simulations reveal that the energetic route of CO oxidation in H2 for Pt/CoO is more active than that for a Pt/Co3O4 surface. [ABSTRACT FROM AUTHOR]

Published
2020
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98. In situ depth‐resolved synchrotron radiation X‐ray spectroscopy study of radiation‐induced Au deposition.

Author

Chen, Guang, Du, Yonghua, An, Pengfei, Zheng, Lirong, Chu, Shengqi, and Zhang, Jing

Subjects
X-ray spectroscopy, SYNCHROTRON radiation, CHEMICAL species, X-ray imaging, RADIOLYSIS
Abstract

To illustrate the process of synchrotron radiation induced reduction of tetrachloroauric solutions, a confocal synchrotron radiation X‐ray spectroscopy experiments system has been introduced to monitor the depth‐resolved elemental Au distribution and chemical species during the Au reduction reaction. Combining the results from confocal X‐ray spectroscopy with that from X‐ray contrast imaging, the mechanism of synchrotron radiation induced Au reduction, along with the process of Au deposition, were proposed. These demonstrations provide novel avenues to spatially resolved analysis of in situ solution radiolysis. [ABSTRACT FROM AUTHOR]

Published
2019
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