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Tandem Catalysis for Selective Oxidation of Methane to Oxygenates Using Oxygen over PdCu/Zeolite

Angewandte Chemie 2022年第24期134卷

作者： Bo Wu Tiejun Lin Min Huang Shenggang Li Ji Li Xing Yu Ruoou Yang Fanfei Sun Zheng Jiang Yuhan Sun Liangshu Zhong CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China School of Physical Science and Technology ShanghaiTech University Shanghai 201210 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China

Selective oxidation of methane to oxygenates with O 2 under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O 2 in the presence of H 2 at low temperature (120 °C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g −1 Pd h −1 (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %. Control experiments and mechanistic studies revealed that PdO nanoparticles promoted the in situ generation of H 2 O 2 from O 2 and H 2 , while Cu single atoms not only accelerated the activation of H 2 O 2 for the generation of abundant hydroxyl radicals (⋅OH) from H 2 O 2 decomposition, but also enabled the homolytic cleavage of CH 4 by ⋅OH to methyl radicals (⋅CH 3 ). Subsequently, the ⋅OH reacted quickly with the ⋅CH 3 to form CH 3 OH with high selectivity.

关键词： Methane Oxygenates Reaction Mechanisms Selective Oxidation Tandem Catalysis

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2020 Roadmap on gas-involved photo-and electro-catalysis

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Chinese Chemical Letters 2019年第12期30卷 2089-2109页

作者： Yulu Yang Yang Tang Haomin Jiang Yongmei Chen Pingyu Wan Maohong Fan Rongrong Zhang Sana Ullah Lun Pan Ji-Jun Zou Mengmeng Lao Wenping Sun Chao Yang Gengfeng Zheng Qiling Peng Ting Wang Yonglan Luo Xuping Sun Alexander S.Konev Oleg V.Levin Panagiotis Lianos Zhuofeng Hu Zhurui Shen Qinglan Zhao Ying Wang Nadia Todorova Christos Trapalis Matthew V.Sheridan Haipeng Wang Ling Zhang Songmei Sun Wenzhong Wang Jianmin Ma School of Physics and Electronics Hunan UniversityChangsha 410082China College of Chemistry Beijing University of Chemical TechnologyBeijing 100029China School of Civil and Environmental Engineering Georgia Institute of TechnologyAtlantaGA 30332United States College of Engineering and Applied Sciences and School of Energy ResourcesUniversity of WyomingLaramieWY 82071United States Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongNSW 2522Australia Laboratory of Advanced Materials Department of ChemistryFudan UniversityShanghai 200438China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China Institute of Chemistry St.Petersburg State University7/9 Universitetskaya emb.St.Petersburg 199034Russian Federation Department of Chemical Engineering University of PatrasPatras 26500Greece School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation TechnologySun Yat-sen UniversityGuangzhou 510275China School of Materials Science and Engineering Nankai UniversityTianjin 300350China Department of Chemistry Chinese University of Hong KongHong KongChina Institute of Nanoscience and Nanotechnology NCSR"Demokritos"Athens 15341Greece State Key Laboratory of School of Radiation Medicine and Protection and School for Radiological and interdisciplinary Sciences(RAD-X) Soochow UniversitySuzhou 215123China State Key Laboratory of High Performance Ceramics and Superf

Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal ***-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright ***,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) *** can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction ***,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction ***,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble *** reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted *** them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of ***,the cost,synthetic methods of catalysts should also be ***,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so *** extremely active fields,we should pay attention to *** the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.

关键词： H2 evolution reaction O2 reduction reaction O2 evolution reaction CO2 reduction reaction N2 reduction reaction Electrocatalysis Photocatalysis Photoelectrocatalysis

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FeVO 4 ⋅nH 2 [email protected] nanocomposite as high performance cathode materials for aqueous Zn-ion batteries

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Journal of Alloys and Compounds 2020年 818卷

作者： Binxu Lan Chen Tang Lineng Chen Wenwei Zhang Wen Tang Chunli Zuo Xudong Fu Shijie Dong Qinyou An Ping Luo Hubei Provincial Key Laboratory of Green Materials for Light Industry Collaborative Innovation Center of Green Light-Weight Materials and Processing School of Materials and Chemical Engineering Hubei University of Technology Hubei Wuhan 430068 PR China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Hubei University of Economics Hubei Wuhan 430205 PR China

Aqueous zinc ion batteries (ZIBs) have recently attracted an increasing attention as an environmental friendliness, low cost and highly potential novel energy storage system. Although vanadium-based materials serve as a capable of arousing and holding the attention cathode materials for ZIBs, whereas low conductivity and confusing zinc ion storage mechanisms remain an obstacle. Herein, FeVO 4 ⋅nH 2 [email protected] composite is employed to evaluate zinc ion storage capability as a cathode for the first time in 2 M Zn(TFSI) 2 electrolyte. Benefiting from the large lattice spacing, dual electrochemical activity and fast electron transfer, the composite delivers excellent rate performance and long life cycle (the capacity retained ∼100 mAh g −1 at 1.0 A g −1 after 1000 cycle). In addition, the electrochemical performance of graphene-modified FeVO 4 ⋅nH 2 O is superior to other precursors for comparison. Furthermore, the intercalated/de-intercalated mechanism of zinc ion is distinct from the traditional conversion reaction, which is confirmed by in-situ X-ray diffraction and various ex-situ techniques.

关键词： FeVO 4 ⋅nH 2 [email protected] Aqueous zinc ion batteries Cathode Energy storage mechanism

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Regulating Non-Equilibrium Solvation Structure in Locally Concentrated Ionic Liquid Electrolytes for Wide-Temperature and High-Voltage Lithium Metal Batteries

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Angewandte Chemie 2024年第1期137卷

作者： Haifeng Tu Zhicheng Wang Jiangyan Xue Zhiyong Tang Yang Liu Xiaofang Liu Lingwang Liu Suwan Lu Shixiao Weng Yiwen Gao Guochao Sun Zheng Liu keyang Peng Xin Zhang Dejun Li Guangye Wu Meinan Liu Jianchen Hu Hong Li Jingjing Xu Xiaodong Wu School of Nano-Tech and Nano-Bionics University of Science and Technology of China Hefei Anhui 230026 China i-lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou Jiangsu 215123 China These authors contributed equally to this work: Haifeng Tu Zhicheng Wang Institute of Physics Chinese Academy of Sciences Beijing 100190 China Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang 213300 China Jiangxi Key Laboratory of Flexible Electronics Jiangxi Science & Technology Normal University Nanchang 330013 Jiangxi China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials School of Resources Environment and Materials Guangxi University Nanning 530004 China National Engineering Laboratory for Modern Silk College of Textile and Clothing Engineering Research Center of Cooperative Innovation for Functional Organic/Polymer Material Micro/Nanofabrication Soochow University Suzhou 215123 China College of Material Science and Engineering Hohai University Nanjing Jiangsu 210024 China

The development of high-voltage lithium metal batteries (LMBs) encounters significant challenges due to aggressive electrode chemistry. Recently, locally concentrated ionic liquid electrolytes (LCILEs) have garnered attention for their exceptional stability with both Li anodes and high-voltage cathodes. However, there remains a limited understanding of how diluents in LCILEs affect the thermodynamic stability of the solvation structure and transportation dynamics of Li + ions. Herein, we propose a wide-temperature LCILEs with 1,3-dichloropropane (DCP13) diluent to construct a non-equilibrium solvation structure under external electric field, wherein the DCP13 diluent enters the Li + ion solvation sheath to enhance Li + ion transport and suppress oxidative side reactions at high-nickel cathode (LiNi 0.9 Co 0.05 Mn 0.05 O 2 , NCM90). Consequently, a Li/NCM90 cell utilizing this LCILE achieves a high capacity retention of 94 % after 240 cycles at 4.3 V, also operates stably at high cut-off voltages from 4.4 V to 4.6 V and over a wide temperature range from −20 °C to 60 °C. Additionally, an Ah-level pouch cell with this LCILE simultaneously achieves high-energy-density and stable cycling, manifesting the practical feasibility. This work redefines the role of diluents in LCILEs, providing inspiration for electrolyte design in developing high-energy-density batteries.

关键词： Lithium metal batteries locally concentrated ionic liquid electrolyte chloroalkane diluent non-equilibrium solvation structure external electric field

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Energy storage through intercalation reactions: electrodes for rechargeable batteries

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National Science Review 2017年第1期4卷 26-53页

作者： Robert C.Massé Chaofeng Liu Yanwei Li Liqiang Mai Guozhong Cao Department of Materials Science and Engineering University of Washington State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Guangxi Key Laboratory of Electrochemical and Magneto-Chemical Functional Materials College of Chemistry and BioengineeringGuilin University of Technology

Electrochemical energy storage has been an important enabling technology for modern electronics of all kinds,and will grow in importance as more electric vehicles and grid-scale storage systems are *** briely review the history of intercalation electrodes and basic concepts pertaining to bateries based on intercalation *** we summarize how the critical performance metrics—energy density,power density,safety and stability—relate back to electrode materials properties,and how these materials properties are related to fundamental chemical and physical structure relationships highlighted with the most recent research *** and avenues for further research have been highlighted throughout.

关键词： intercalation rechargeable bateries energy density power density stability safety

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Regulative Electronic states around Ruthenium/Ruthenium Disulphide Heterointerfaces for Efficient Water Splitting in Acidic Media

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Angewandte Chemie 2021年第22期133卷

作者： Jiawei Zhu Dr. Yao Guo Fang Liu Hanwen Xu Lei Gong Wenjie Shi Ding Chen Pengyan Wang Yue Yang Chengtian Zhang Prof. Jinsong Wu Dr. Jiahuan Luo Prof. Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China Department of Chemical and Environmental Engineering Anyang Institute of Technology Anyang 455000 P. R. China NRC (Nanostructure Research Centre) Wuhan University of Technology Wuhan 430070 P. R. China

Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS 2 heterostructure. The resulting surface electron-deficient Ru sites display optimized adsorption behavior toward diverse reaction intermediates, thereby reducing the thermodynamic energy barriers. Experimentally, for the first time the laminar Ru/RuS 2 heterostructure is rationally engineered by virtue of the synchronous reduction and sulfurization under eutectic salt system. Impressively, it exhibits extremely high catalytic activity for both OER (201 mV @ 10 mA cm −2 ) and HER (45 mV @ 10 mA cm −2 ) in acidic media due to favorable kinetics and excellent specific activity, consequently leading to a terrific performance in acidic overall water splitting devices (1.501 V @ 10 mA cm −2 ). The in-depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.

关键词： acidic water electrolysis bifunctional electrocatalyst DFT calculation heterostructure Ru-based nanomaterial

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Oxygen self-doped g-C3N4 with tunable electronic band structure for unprecedentedly enhanced photocatalytic performance

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Nanoscale 2018年第9期10卷 4515-4522页

作者： Fangyan Wei Yang Liu Heng Zhao Xiaoning Ren Jing Liu Tawfique Hasan Lihua Chen Yu Li Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China. yu.li@***.

As a fascinating conjugated polymer, graphitic carbon nitride (g-CN) has attracted much attention for solving the worldwide energy shortage and environmental pollution. In this work, for the first time we report oxygen self-doping of solvothermally synthesized g-CN nanospheres with tunable electronic band structure via ambient air exposure for unprecedentedly enhanced photocatalytic performance. Various measurements, such as XPS, Mott-Schottky plots, and density functional theory (DFT) calculations reveal that such oxygen doping can tune the intrinsic electronic state and band structure of g-CNvia the formation of C-O-C bond. Our results show that the oxygen doping content can be controlled by the copolymerization of the precursors. As a consequence, the oxygen doped g-CN shows excellent photocatalytic performance, with an RhB photodegradation rate of 0.249 min and a hydrogen evolution rate of 3174 μmol h g, >35 times and ∼4 times higher than that of conventional thermally made pure g-CN (0.007 min and 846 μmol h g, respectively) under visible light. Our work introduces a new route for the rational design and fabrication of doping modified g-CN photocatalyst for efficient degradation of organic pollutants and H production.

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Insight into the positive effect of porous hierarchy in S/C cathodes on the electrochemical performance of Li-S batteries

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Nanoscale 2018年第25期10卷 11861-11868页

作者： Pan Wu Li-Hua Chen Shan-Shan Xiao Shen Yu Zhao Wang Yu Li Bao-Lian Su Laboratory of Living Materials the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan China. chenlihua@*** zhao.wang@***.

Hierarchically porous carbon-supported sulfur material is widely used as a cathode for Li-S batteries because its large surface area and rich porous system provide high sulfur loading, resulting in high specific capacity with stable charge/discharge cycling performance. However, limited attention has been paid to whether the structure of hierarchical porous system affects the final electrochemical performance of Li-S/C batteries. Herein, we present hierarchically structured carbon (WSAC) with varied amounts of mesopores and micropores as a sulfur container for Li-S batteries. It is found that the relationship between electrochemical performance and percentage of microporous volume obeys a volcano distribution, which indicates that the volume percentage of microporous in the meso-microporous structure could be suitably tuned to achieve the desired electrochemical performance. Such S/hierarchically meso-microporous carbon (i.e., WSAC-8) with moderate microporous volume percentage (68.3%) shows high initial specific capacity (1375 mA h g-1) and stable charge/discharge performance (942.6 mA h g-1 after 200 cycles at 0.5C). In particular, WSAC-8 also presented superior capacity behavior at high rate capability, with final capacity as high as 800.1 and 758.7 mA h g-1 for 1C and 2C, respectively.

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Fabrication of Efficient and Stable Perovskite Solar Cells in High-Humidity Environment through Trace-Doping of Large-Sized Cations

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ChemSusChem 2019年

作者： Liu, Xueping He, Jiang Wang, Pengfei Liu, Yuhao Xiao, Junyan Ku, Zhiliang Peng, Yong Huang, Fuzhi Cheng, Yi-Bing Zhong, Jie State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan430074 China School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China Department of Materials Science and Engineering Monash University VIC3800 Australia ARC Centre of Excellence in Exciton Science Monash University ClaytonVIC3800 Australia

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Effect of Hot Pressure Parameters on W-SiC/Cu Composites Densification

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IOP Conference Series: materials Science and Engineering 2019年第1期678卷

作者： Chengcheng Zhang Qiang Shen Jian Zhang Guoqiang Luo Yi Sun Yuan Li Lianmeng Zhang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China

In the paper, 30W-30SiC/40wt.%Cu composites were fabricated by tape casting and hot-pressing sintering. Microstructures of the W-SiC/Cu green tape and the green tape after organic additives removal were studied. The results showed that W, Cu and SiC particles exhibited a uniform distribution. The effects of sintering temperature, sintering pressure and holding time on the microstructures, porosity, and density of the W-SiC/Cu composites were investigated. The results showed the porosity of the W-SiC/Cu composites decreased and the density increased with the increasing of the sintering temperature, sintering pressure and holding time. The porosity and density of the W-SiC/Cu composite prepared at the condition of 900 °C- 200 MPa- 2 h achieved 0.52 % and 9.84 g/cm3.

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