Article
Engineering, Environmental
Tong Shi, Dong Liu, Hao Feng, Ying Zhang, Qiang Li
Summary: This study investigates the evolution of electrode surface and CO2RR performance after surface modifications. The results show that the modified copper electrode forms a stable triple-phase interface, resulting in enhanced current density and reduced H2 production.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Lingzhi Sun, Zhaoyu Zhou, Yanan Xie, Jingui Zheng, Xun Pan, Lina Li, Guohua Zhao
Summary: DFT calculations are used to adjust the local coordination environment and electronic structure of Ni3S2 by Fe doping, promoting the self-reconstruction of catalyst and improving the nitrile evolution reaction performance. Benzylamine electrooxidation coupled with hydrogen production achieved a 14.5-fold improvement in hydrogen production compared to water electrolysis, converting benzylamine to high-value benzonitrile with a 99% product yield. Fe doping induced surface self-reconstruction of Ni3S2 to NiOOH, reducing the energy barriers for C-N bonds to C(sic)N bonds.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Lei Lv, Ruihu Lu, Jiexin Zhu, Ruohan Yu, Wei Zhang, Enhui Cui, Xingbao Chen, Yuhang Dai, Lianmeng Cui, Jiong Li, Liang Zhou, Wei Chen, Ziyun Wang, Liqiang Mai
Summary: In this study, a catalyst with excellent selectivity for electrocatalytic CO2 reduction reaction (ECO2RR) and inhibition of competing hydrogen evolution reaction (HER) has been developed by coordinating the edge defects of bismuth (Bi) with sulfur. The catalyst exhibits high product selectivity, with a HCOO- Faraday efficiency of approximately 95% and an HCOO- partial current of approximately 250 mA cm(-2) under alkaline electrolytes. Density function theory calculations reveal the mechanism behind the improved selectivity and provide guidance for the design of advanced ECO2RR catalysts based on bismuth.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jiao Liu, Peng Ding, Zexuan Zhu, Wei Du, Xiaoyong Xu, Jingguo Hu, Yong Zhou, Haibo Zeng
Summary: Transition metal-based catalysts undergo surface reconstruction to generate active sites for high OER performance. This study proposes using self-reconstruction as an efficient strategy to develop novel OER catalysts by designing pre-catalysts with flexible components susceptible to OER conditions. By constructing NiFe-based LDHs intercalated with MoO42- anions and achieving complete ECSR into active NiFeOOH, the catalyst showed excellent OER performance and durability, indicating the potential of ECSR engineering in component-flexible precursors for developing highly active OER catalysts.
Article
Chemistry, Physical
Tong Wu, Zian Xu, Xunlu Wang, Mengjia Luo, Yu Xia, Xingcai Zhang, Jiantao Li, Jie Liu, Jiacheng Wang, Hsing-Lin Wang, Fuqiang Huang
Summary: In this study, a self-confined surface reconstruction strategy is proposed to construct NiOOH layers with superior activity and stability for biomass electro-oxidation. The strategy effectively prevents in-depth surface oxidation and enhances electron transfer kinetics, resulting in high reaction conversion and selectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Chang Liu, Xiang-Da Zhang, Jian-Mei Huang, Meng-Xue Guan, Ming Xu, Zhi-Yuan Gu
Summary: In this study, highly active Cu/Cu2O nanoclusters were successfully synthesized via in situ electrochemical reconstruction for the highly selective synthesis of C2H4 in CO2 electroreduction. The coexistence of Cu2O and Cu nanoclusters as active sites was confirmed by in situ infrared spectroscopy and Raman spectroscopy.
Article
Chemistry, Physical
Lian Ma, Qinghong Geng, Longlong Fan, Jun-Xuan Li, Dawei Du, Junli Bai, Cuiling Li
Summary: Polyaniline/CuO nanosheets (PANI/CuO NSs) hybrid electrocatalysts are developed to achieve superior C2+ selectivity by electrochemically converting CO2 to value-added multi-carbon (C2+) fuels and chemicals.
Article
Multidisciplinary Sciences
Shuo Zhang, Miao Li, Jiacheng Li, Qinan Song, Xiang Liu
Summary: Metal-organic framework-derived cobalt-doped Fe@Fe2O3 catalyst shows high efficiency in electrochemical nitrate reduction and ammonia production, providing an important strategy in the design of electrocatalysts.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Jing Wang, Jing Hu, Siqi Niu, Siwei Li, Yunchen Du, Ping Xu
Summary: This article reports an efficient bifunctional electrocatalyst for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline solution. The catalyst exhibits good performance at both low and overpotentials, and demonstrates outstanding long-term durability. Spectroscopic studies reveal the importance of in situ surface reconstruction for the enhanced catalytic activity in both HER and OER processes.
Article
Chemistry, Applied
Na Zhou, Jiazhi Wang, Ning Zhang, Zhi Wang, Hengguo Wang, Gang Huang, Di Bao, Haixia Zhong, Xinbo Zhang
Summary: In this study, a copper and copper-tetracyanoquinodimethane composite catalyst (Cu@CuTCNQ) with high density of copper vacancy defects was developed. The catalyst showed efficient electrocatalytic reduction of nitrate to ammonia (NRA) through an in situ electrochemical reconstruction method. The Cu@CuTCNQ exhibited superior catalytic performance for NRA, with high Faradaic efficiency and productivity, due to the synergistic effect of copper vacancy defects and interfacial charge transfer.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Jie Zhang, Thi Ha My Pham, Zhixiao Gao, Mo Li, Youngdon Ko, Loris Lombardo, Wen Zhao, Wen Luo, Andreas Zuttel
Summary: Metal complexes have been found to be selective and active catalysts for electrochemical CO2 reduction (CO2RR). Using in situ Raman, X-ray photoelectron spectroscopy, and advanced electron microscopy, researchers have discovered that copper phthalocyanine (CuPc) undergoes reconstruction during CO2RR. Further investigations have revealed that CuPc demetalates to Cu atoms, which then agglomerate to form Cu clusters and Cu nanoparticles (NPs). The size of the Cu NPs is highly dependent on experimental parameters, and the selectivity of multicarbon products is positively correlated with NP size. This study provides important insights for future applications of metal complex catalysts in CO2RR and inspires the design of advanced electrocatalysts for other electrochemical reactions.
Article
Multidisciplinary Sciences
Jiarui Yang, Wen-Hao Li, Hai-Tao Tang, Ying-Ming Pan, Dingsheng Wang, Yadong Li
Summary: The chlor-alkali process generates chlorine and sodium hydroxide through the electrolysis of sodium chloride solutions, which are important for chemical manufacturing. Despite being an energy-intensive process, with a significant portion of global electricity production going towards it, there is still a need for a new electrocatalyst to improve efficiency in the chlorine evolution reaction.
Article
Engineering, Environmental
Shihao Zhou, Junwen Zhu, Zunrui Wang, Zhen Yang, Weiben Yang, Zhonglong Yin
Summary: A novel anodic membrane has been developed for the coupling of electro-oxidation and membrane filtration process in municipal wastewater reclamation. This membrane demonstrates excellent anti-fouling and self-cleaning abilities, efficient removal of antibiotics and bactericidal efficiency without the need for chemical reagents. It also presents excellent stability, separation performance and low energy consumption, providing a promising solution for wastewater reclamation.
Article
Chemistry, Physical
Daniel Arenas Esteban, Lien Pacquets, Daniel Choukroun, Saskia Hoekx, Ajinkya Anil Kadu, Jonathan Schalck, Nick Daems, Tom Breugelmans, Sara Bals
Summary: The increasing use of metallic nanoparticles is advancing electrocatalysis, specifically in the field of electrochemical CO2 reduction reaction. This study investigates the structural transformation mechanism of Cu@Ag core-shell nanoparticles during the critical first minutes of the reaction. The research findings provide insights into how bimetallic core-shell nanoparticles transform under electrochemical conditions.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Jiayi Zhong, Qiming Chen, Caixia Guo, Wenchao Peng, Yang Li, Fengbao Zhang, Xiaobin Fan
Summary: Transition metal Co-based materials, such as layered double hydroxides (LDHs), can undergo electrochemical reconstruction under oxygen evolution reaction (OER) conditions to form highly active Co4 species. However, controlling the formation of these species remains challenging. In this study, the leaching of Al3 after OER activation successfully induces the formation of high-valent Co4 species on CoFeAl LDH, leading to an electrocatalyst with excellent OER performance. This work provides insights into surface reconstruction and activity promotion using leachable cations to induce high-valent metal active sites in other electrocatalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Letter
Materials Science, Multidisciplinary
Qi Liu, Meng-Yang Li, Yan-Mei Shi, Cui-Bo Liu, Yi-Fu Yu, Bin Zhang
Article
Chemistry, Physical
Yanmei Huang, Rong Yang, Changhong Wang, Nannan Meng, Yanmei Shi, Yifu Yu, Bin Zhang
Summary: Electrochemical synthesis of urea is a sustainable strategy that utilizes abundant and low-cost inorganic carbon and nitrogen sources through advanced electrocatalytic processes to achieve efficient urea generation.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Shanshan Lu, Wei Zhou, Yanmei Shi, Cuibo Liu, Yifu Yu, Bin Zhang
Summary: This study successfully develops a cheap and efficient acidic OER material by transforming inexpensive graphite flakes into functionalized graphite MEO-GP through MEO treatment. Multiple characterizations reveal that PQ-like moiety is the most active species for acidic OER.
Article
Multidisciplinary Sciences
Ying Gao, Rong Yang, Changhong Wang, Cuibo Liu, Yongmeng Wu, Huizhi Li, Bin Zhang
Summary: Efficient and selective electrocatalytic alkyne semihydrogenation is achieved by sulfur-tuned effects and field-induced reagent concentration. The study reveals the role of sulfur anions and electric field in promoting the reaction.
Article
Chemistry, Multidisciplinary
Yuting Wang, Hongjiao Li, Wei Zhou, Xi Zhang, Bin Zhang, Yifu Yu
Summary: Carbon-supported RuO2 nanosheets with adjustable crystallinity show high efficiency and selectivity in nitrate reduction to ammonia, outperforming crystalline counterparts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Tieliang Li, Shuhe Han, Chuanqi Cheng, Yuting Wang, Xiwen Du, Yifu Yu, Bin Zhang
Summary: The electrocatalytic nitrogen oxidation reaction (NOR) has gained attention as an alternative method for the production of nitrate. By using sulfate, the performance of NOR on a Rh electrocatalyst was enhanced, resulting in a higher nitrate yield. Experimental and theoretical studies revealed that sulfate promoted nitrogen adsorption, decreased reaction energy barriers, and accelerated the NOR process through the formation of sulfate radicals.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Shuyan Han, Chuanqi Cheng, Meng He, Rui Li, Ying Gao, Yifu Yu, Bin Zhang, Cuibo Liu
Summary: A green and efficient electrosynthesis method for ethylene chlorohydrin (ECH) was developed using NaCl as a catalyst over a NiFe2O4 nanosheet anode from ethylene oxide (EO). The adsorption of EO and Cl on Fe and Ni sites, respectively, promoted the ECH synthesis. A Cl radical-mediated ring-opening process was proposed and confirmed, and key Cl and carbon radical species were identified. This strategy allowed for scalable electrosynthesis of ECH with high yield and also showed potential for the synthesis of other chloro- and bromoethanols.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Huaifang Zhang, Yanbo Li, Chuanqi Cheng, Jin Zhou, Pengfei Yin, Haoming Wu, Zhiqin Liang, Jiangwei Zhang, Qinbai Yun, An-Liang Wang, Lijie Zhu, Bin Zhang, Wenbin Cao, Xiangmin Meng, Jing Xia, Yifu Yu, Qipeng Lu
Summary: The direct electrochemical nitric oxide reduction reaction (NORR) is an attractive technique for converting NO into NH3 with low power consumption under ambient conditions. Optimizing the electronic structure of the active sites can greatly improve the performance of electrocatalysts. In this study, body-centered cubic RuGa intermetallic compounds (bcc RuGa IMCs) were prepared via a substrate-anchored thermal annealing method. The electrocatalyst showed a remarkable NH4+ yield rate of 320.6 mu mol h(-1) mg(Ru)(-1) with a corresponding Faradaic efficiency of 72.3% at a very low potential of -0.2 V vs. reversible hydrogen electrode (RHE) in neutral media. Theoretical calculations revealed that the electron-rich Ru atoms in bcc RuGa IMCs facilitated the adsorption and activation of *HNO intermediate, thus greatly reducing the energy barrier of the potential-determining step in NORR.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Bingyi Lu, Biao Chen, Dashuai Wang, Chuang Li, Runhua Gao, Yingqi Liu, Rui Mao, Jinlong Yang, Guangmin Zhou
Summary: A bidirectional catalyst V-MoS2/Co9S8@CP has been designed, which vertically grows MoS2 and Co9S8 on carbon paper to provide abundant edge active sites, improve interfacial conductivity, and modulate electron transport along the basal planes. This catalyst shows superior performance in CO2RR and CO2ER compared to other catalysts. This work not only provides insights into the rational design of electronic contact in transition metal dichalcogenides with specified crystal facets, but also guides the design of high-performance cathodic catalysts in Li-CO2 batteries.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Review
Chemistry, Multidisciplinary
Cuibo Liu, Yongmeng Wu, Bohang Zhao, Bin Zhang
Summary: The electrocatalytic hydrogenation using water as the hydrogen source offers an efficient and sustainable approach to synthesize hydrogenated products. Utilizing heavy water for deuterated syntheses is also attractive due to the widespread applications of deuterated molecules. However, the rational design of nanostructured electrodes for driving the electrocatalytic hydrogenation and understanding the reaction outcomes are still challenging.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Multidisciplinary Sciences
Shanshan Lu, Chuanqi Cheng, Yanmei Shi, Yongmeng Wu, Zhipu Zhang, Bin Zhang
Summary: Heteroatom-doped carbon materials are widely used in electrocatalytic reduction reactions. However, their structural evolution and active origins are often ignored.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Physical
Bohang Zhao, Fanpeng Chen, Chuanqi Cheng, Li Li, Cuibo Liu, Bin Zhang
Summary: Constructing Cu-0-Cu+ double-active sites is important for C-C coupling in CO2 electrocatalytic reduction, but stabilizing Cu+ is challenging. In this study, fullerene (C-60) is used to stabilize Cu+ and a composite of copper oxide and C-60 precursor is designed to obtain a catalyst with Cu-0-Cu+ double-active sites. The catalyst shows high multicarbon product selectivity and good stability.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Shuhe Han, Hongjiao Li, Tieliang Li, Fanpeng Chen, Rong Yang, Yifu Yu, Bin Zhang
Summary: Ammonia plays a crucial role in agriculture and carbon-free energy supply. A three-step relay mechanism is proposed to enhance the energy efficiency of electrocatalytic nitrate reduction to ammonia. By designing RuCo alloys as catalysts, high-performance ammonia production with low cost has been achieved.
Article
Green & Sustainable Science & Technology
Bo-Hang Zhao, Fanpeng Chen, Mengke Wang, Chuanqi Cheng, Yongmeng Wu, Cuibo Liu, Yifu Yu, Bin Zhang
Summary: The authors demonstrate a rationally designed Cu catalyst for electrocatalytic production of ethylene, which shows high performance, economic feasibility, and sustainability.
NATURE SUSTAINABILITY
(2023)
Article
Chemistry, Physical
Mengyang Li, Yongmeng Wu, Bo-Hang Zhao, Chuanqi Cheng, Jinghui Zhao, Cuibo Liu, Bin Zhang
Summary: A sustainable electrocatalytic method for the synthesis of alanine from NO and pyruvic acid over oxide-derived Ag is reported. A decoupled electrosynthesis system is designed, delivering easily purified alanine with high efficiency. This method has potential for solar-energy-driven alanine synthesis and the fabrication of other amino acids.