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Cascade Electrocatalytic and Thermocatalytic Reduction of CO2to Propionaldehyde

Angewandte Chemie 2024年第12期136卷

作者： Jie Zhang Xingsi Kang Yuchen Yan Xue Ding Prof. Lin He Prof. Yanguang Li Institute of Functional Nano and Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICP Lanzhou Institute of ChemicalPhysics (LICP) Chinese Academy of Sciences Lanzhou 730000 China Macao Institute of Materials Science and Engineering (MIMSE) MUST-SUDA Joint Research Center for Advanced Functional Materials Macau University of Science and Technology Taipa Macao 999078 China

Electrochemical CO 2 reduction can convert CO 2 to value-added chemicals, but its selectivity toward C 3+ products are very limited. One possible solution is to run the reactions in hybrid processes by coupling electrocatalysis with other catalytic routes. In this contribution, we report the cascade electrocatalytic and thermocatalytic reduction of CO 2 to propionaldehyde. Using Cu(OH) 2 nanowires as the precatalyst, CO 2 /H 2 O is reduced to concentrated C 2 H 4 , CO, and H 2 gases in a zero-gap membrane electrode assembly (MEA) reactor. The thermochemical hydroformylation reaction is separately investigated with a series of rhodium-phosphine complexes. The best candidate is identified to be the one with the 1,4-bis(diphenylphosphino)butane diphosphine ligand, which exhibits a propionaldehyde turnover number of 1148 under a mild temperature and close-to-atmospheric pressure. By coupling and optimizing the upstream CO 2 electroreduction and downstream hydroformylation reaction, we achieve a propionaldehyde selectivity of ~38 % and a total C 3 oxygenate selectivity of 44 % based on reduced CO 2 . These values represent a more than seven times improvement over the best prior electrochemical system alone or over two times improvement over other hybrid systems.

关键词： Cascade catalysis electrochemical CO2 reduction hydroformylation reaction propionaldehyde

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Selective and effective adsorption of cesium ions by metal hexacyanoferrates (MHCF, M = Cu, Co, Ni) modified chitosan fibrous biosorbent

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The Science of the total environment 2022年 835卷 155575页

作者： Shuting Zhuang Kunkun Zhu Jun Hu Jianlong Wang Laboratory of Environmental Technology INET Tsinghua University Beijing 100084 PR China. State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 PR China. Laboratory of Environmental Technology INET Tsinghua University Beijing 100084 PR China Beijing Key Laboratory of Radioactive Waste Treatment INET Tsinghua University Beijing 100084 PR China. Electronic address: wangjl@***.

Selective and effective adsorptive removal of radiocesium is of great importance in terms of nuclear waste management and environmental remediation, but is still challenging because of its radioactive and non-complexing nature. Herein, metal hexacyanoferrates (MHCF, M = Cu, Co, or Ni) modified fibrous chitosan was prepared by multiple sequential adsorption and self-assembly approach, and applied for the selective and effective adsorption of Cs. The physically supported MHCF in chitosan fibers showed good crystallinity and stability, and the obtained fibrous composite has high specific surface area (18.2-29.4 m g). Moreover, MHCF crystals endowed the fibrous chitosan-based adsorbent with a high adsorption capacity and selectivity towards Cs. Its adsorption kinetic and isotherm performance followed the pseudo second-order model and the Sips model. The q value of three fibrous MHCF/chitosan (M = Cu, Co, or Ni) composites was 24.9-70.3 mg g. The fibrous CuHCF/chitosan composite had the highest q among the three composites. In summary, the modified chitosan can selectively and effectively remove Cs from complicated aqueous solutions.

关键词： Adsorption Biosorbent Cesium ions Chitosan Metal hexacyanoferrates

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Functional Aqueous Zinc–Acetylene Batteries for Electricity Generation and Electrochemical Acetylene Reduction to Ethylene

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Angewandte Chemie 2022年第12期134卷

作者： Siying An Zhenpeng Liu Jun Bu Jin Lin Yuan Yao Chen Yan Prof. Wei Tian Prof. Jian Zhang Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology Department of Advanced Chemical Engineering School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an Shaanxi 710000 P. R. China State Key Laboratory of Solidification Processing and School of Materials Science and Engineering Northwestern Polytechnical University Xi'an Shaanxi 710072 P. R. China

The available processes for removing acetylene impurities from crude ethylene are tremendously energy-intensive. Herein, we demonstrate a novel aqueous Zn–C 2 H 2 battery, which not only switches energy-consuming acetylene removal to electricity generation, but also reduces acetylene to ethylene through a unique discharge mechanism: C 2 H 2 +Zn+H 2 O→C 2 H 4 +ZnO. Under a pure acetylene stream, this Zn–C 2 H 2 battery exhibits an open circuit potential of 1.14 V and a peak power density of 2.2 mW cm −2 , which exceed those of reported Zn–CO 2 batteries. Even for simulated crude ethylene, the Zn–C 2 H 2 battery manifests an acetylene conversion of 99.97 % and continuously produces polymer-grade ethylene with only ≈3 ppm acetylene during a long-term discharge operation. Such a functional battery is universally appliable for reducing other alkynes and generating electricity. Therefore, this work provides an effective strategy for green ethylene purification and the design of functional batteries.

关键词： Acetylene Semihydrogenation Cu Dendrites Electrocatalysis Ethylene Purification Zn–Acetylene Battery

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Multi-Functional Formaldehyde-Nitrate Batteries for Wastewater Refining, Electricity Generation, and Production of Ammonia and Formate

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Angewandte Chemie 2024年第11期136卷

作者： Siying An Zhi-Hao Zhao Jun Bu Jiaxin He Wenxiu Ma Jin Lin Rui Bai Prof. Li Shang Prof. Jian Zhang State Key Laboratory of Solidification Processing School of Materials Science and Engineering Northwestern Polytechnical University Xi'an Shaanxi 710000 P. R. China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology Department of Advanced Chemical Engineering School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an Shaanxi 710000 P. R. China

As bulky pollutants in industrial and agricultural wastewater, nitrate and formaldehyde pose serious threats to the human health and ecosystem. Current purification technologies including chemical and bio-/photo-/electro-chemical methods, are generally high-cost, time-consuming, or energy-intensive. Here, we report a novel formaldehyde-nitrate battery by pairing anodic formaldehyde oxidation with cathodic nitrate reduction, which simultaneously enables wastewater purification, electricity generation, and the production of high-value-added ammonia and formate. As a result, the formaldehyde-nitrate battery remarkably exhibits an open-circuit voltage of 0.75 V, a peak power density of 3.38 mW cm −2 and the yield rates of 32.7 mg h −1 cm −2 for ammonia and 889.4 mg h −1 cm −2 for formate. In a large-scale formaldehyde-nitrate battery (25 cm 2 ), 99.9 % of nitrate and 99.8 % of formaldehyde are removed from simulated industrial wastewater and the electricity of 2.03 W⋅h per day is generated. Moreover, the design of such a multi-functional battery is universally applicable to the coupling of NO 3 − or NO 2 − reduction with various aldehyde oxidization, paving a new avenue for wastewater purification and chemical manufacturing.

关键词： wastewater purification multi-functional battery nitrate reduction formaldehyde oxidation ammonia production

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Reversible Zn Metal Anodes Enabled by Trace Amounts of Underpotential Deposition Initiators

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Angewandte Chemie 2023年第18期135卷

作者： Yuhang Dai Chengyi Zhang Wei Zhang Lianmeng Cui Chumei Ye Xufeng Hong Jinghao Li Ruwei Chen Wei Zong Xuan Gao Jiexin Zhu Peie Jiang Qinyou An Prof. Dan J. L. Brett Prof. Ivan P. Parkin Dr. Guanjie He Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Christopher Ingold Laboratory Department of Chemistry University College London London WC1H 0AJ UK Electrochemical Innovation Lab Department of Chemical Engineering University College London London WC1E 7JE UK Institute of Technological Sciences Wuhan University Wuhan 430072 P. R. China Department of Materials Science and Metallurgy University of Cambridge Cambridge CB3 0FS UK Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials School of Materials Science and Engineering Peking University Beijing 100871 P. R. China

Routine electrolyte additives are not effective enough for uniform zinc (Zn) deposition, because they are hard to proactively guide atomic-level Zn deposition. Here, based on underpotential deposition (UPD), we propose an “escort effect” of electrolyte additives for uniform Zn deposition at the atomic level. With nickel ion (Ni 2+ ) additives, we found that metallic Ni deposits preferentially and triggers the UPD of Zn on Ni. This facilitates firm nucleation and uniform growth of Zn while suppressing side reactions. Besides, Ni dissolves back into the electrolyte after Zn stripping with no influence on interfacial charge transfer resistance. Consequently, the optimized cell operates for over 900 h at 1 mA cm −2 (more than 4 times longer than the blank one). Moreover, the universality of “escort effect” is identified by using Cr 3+ and Co 2+ additives. This work would inspire a wide range of atomic-level principles by controlling interfacial electrochemistry for various metal batteries.

关键词： Aqueous Battery Electrolyte Additive Interfacial Electrochemistry Underpotential Deposition Zinc Anode

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Cover Feature: Ultrasensitive, Sustainable, and Selective Electrochemical Hydrazine Detection by ALD-Developed Two-Dimensional WO3(ChemElectroChem 2/2018)

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ChemElectroChem 2017年第2期5卷

作者： Zihan Wei Zhenyin Hai Mohammad Karbalaei Akbari Prof. Jie Hu Lachlan Hyde Prof. Stephen Depuydt Prof. Francis Verpoort Prof. Serge Zhuiykov Ghent University Global Campus Department of Applied Analytical & Physical Chemistry 119 Songdomunhwa-ro Yeonsu-gu Incheon South Korea Micro and Nano System Research Center Key Lab of Advanced Transducers and Intelligent Control System (Ministry of Education) & College of Information Engineering Taiyuan University of Technology Taiyuan 030024 Shanxi PR China Factory of the Future Swinburne University of Technology Hawthorn Australia National Research Tomsk Polytechnic University Lenin Avenue 30 634050 Tomsk Russian Federation Laboratory of Organometallics Catalysis and Ordered Materials State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center for Chemical and Material Engineering Wuhan University of Technology Wuhan P.R. China

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A Microstructured Graphene/Poly(N‐isopropylacrylamide) Membrane for Intelligent Solar Water Evaporation

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Angewandte Chemie 2018年第50期130卷

作者： Panpan Zhang Feng Liu Qihua Liao Houze Yao Hongya Geng Huhu Cheng Chun Li Liangti Qu Key Laboratory for Advanced Materials Processing Technology Ministry of Education of China State Key Laboratory of Tribology Department of Mechanical Engineering Tsinghua University Beijing 100084 P. R. China State Key Laboratory of Nonlinear Mechanics Institute of Mechanics Chinese Academy of Sciences Beijing 100190 China Department of Chemistry Tsinghua University Beijing 100084 P. R. China School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 P. R. China

Intelligent solar water evaporation (iSWE) was achieved with a thermally responsive and microstructured graphene/poly( N ‐isopropylacrylamide) (mG/PNIPAm) membrane. As the solar intensity varies, the water evaporation is tuned through reversible transformations of microstructures reminiscent of the stomatal opening and closing of leaves. Consequently, this mG/PNIPAm membrane displays a high water evaporation rate change (ΔWER) of 1.66 kg m −2 h −1 under weak sunlight (intensity<1 sun) and a low ΔWER of 0.24 kg m −2 h −1 under intense sunlight (1 sun

关键词： Bestrahlung Membranen Polymere Wasserverdampfung

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Titelbild: A Microstructured Graphene/Poly(N‐isopropylacrylamide) Membrane for Intelligent Solar Water Evaporation (Angew. Chem. 50/2018)

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Angewandte Chemie 2018年第50期130卷

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Cover Picture: A Microstructured Graphene/Poly(N-isopropylacrylamide) Membrane for Intelligent Solar Water Evaporation (Angew. Chem. Int. Ed. 50/2018)

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Angewandte Chemie International Edition 2018年第50期57卷

作者： Panpan Zhang Prof. Feng Liu Qihua Liao Houze Yao Hongya Geng Dr. Huhu Cheng Prof. Chun Li Prof. Liangti Qu Key Laboratory for Advanced Materials Processing Technology Ministry of Education of China State Key Laboratory of Tribology Department of Mechanical Engineering Tsinghua University Beijing 100084 P. R. China State Key Laboratory of Nonlinear Mechanics Institute of Mechanics Chinese Academy of Sciences Beijing 100190 China Department of Chemistry Tsinghua University Beijing 100084 P. R. China School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 P. R. China

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Author Correction: Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

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Nature communications 2022年第1期13卷 900页

作者： Yajun Qiu Jian Zhang Jing Jin Jiaqiang Sun Haolin Tang Qingqing Chen Zedong Zhang Wenming Sun Ge Meng Qi Xu Youqi Zhu Aijuan Han Lin Gu Dingsheng Wang Yadong Li Department of Chemistry Tsinghua University Beijing China. College of Chemistry and Materials Engineering Wenzhou University Wenzhou Zhejiang China. zhangjian1209@***. State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing China. State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi China. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China. Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University Wuhu Anhui China. College of Science China Agricultural University Beijing China. swm@***. College of Chemistry and Materials Engineering Wenzhou University Wenzhou Zhejiang China. Research Center of Materials Science Beijing Institute of Technology Beijing China. Institute of Physics Chinese Academy of Sciences Beijing China. Department of Chemistry Tsinghua University Beijing China. wangdingsheng@***.

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