Article
Chemistry, Multidisciplinary
Sheng Dai, Tzu-Hsi Huang, Wei- Liu, Chia-Wei Hsu, Sheng-Wei Lee, Tsan-Yao Chen, Ya-Chen Wang, Jeng-Han Wang, Kuan-Wen Wang
Summary: The electrochemical CO2 reduction reaction serves as a viable alternative to convert intermittent electricity from renewable sources to value-added chemicals. The development of economic catalysts with high efficiency is critical in accelerating CO2 utilization technology. The Au-Cu alloyed core-shell catalyst shows superior performance in CO2-to-CO electrochemical conversion.
Review
Chemistry, Physical
Xulei Sui, Lei Zhang, Junjie Li, Kieran Doyle-Davis, Ruying Li, Zhenbo Wang, Xueliang Sun
Summary: Undoubtedly, noble-metal single atom catalysts (SACs) have become a popular research topic in catalysis due to their low cost, high atomic utilization, and unique performance. Support materials play a crucial role in the preparation and catalytic performance of SACs, leading to rapid development and elaborately designed diverse support materials in recent years. The review systematically introduces the support effects in noble-metal SACs, classifies and discusses the latest advances in support materials, and summarizes design strategies for advanced supports to guide future development and utilization.
ADVANCED ENERGY MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Domenico Grammatico, Andrew J. Bagnall, Ludovico Riccardi, Marc Fontecave, Bao-Lian Su, Laurent Billon
Summary: This review discusses the state of the art of different catalyst-support systems for CO2RR and proposes necessary steps for future developments. The article emphasizes the need for standard benchmarking for comparison of these support systems and the development of advanced techniques to aid rational design principles.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Nanoscience & Nanotechnology
Mingjie Pu, Wanlin Guo, Yufeng Guo
Summary: Using a combination of non-noble metal atoms and defect-engineered transition metal dichalcogenide (TMD) monolayers, new types of single-atom catalysts for electrochemical CO2RR can be designed, exhibiting better catalytic performance and selectivity. Applying suitable biaxial tensile strains on defect-engineered TMDs can significantly reduce the overpotentials of non-noble metal atoms, with the vacancy defects and charge transfer playing a crucial role in improving catalytic activity.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Chemistry, Physical
Zhanzhao Fu, Mingliang Wu, Yipeng Zhou, Zhiyang Lyu, Yixin Ouyang, Qiang Li, Jinlan Wang
Summary: This review provides an overview of recent progress in single-atom catalysts (SACs) for the electrochemical CO2 reduction reaction (CO2RR), focusing on the influence of catalyst supports such as graphene and conjugated macrocycle, as well as factors like heteroatom doping and bimetals on the activity and selectivity of the catalysts. Insights on the intrinsic connection between electronic structures and catalytic properties are summarized, along with discussions on the stability and dynamic structural changes of SACs under operating conditions. Challenges and perspectives for future development of efficient SACs based on graphene and conjugated macrocycle supports are also addressed.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Review
Chemistry, Multidisciplinary
Yuanzhi Zhu, Xiaoxuan Yang, Cheng Peng, Cameron Priest, Yi Mei, Gang Wu
Summary: This passage describes the application of carbon-supported single-atom catalysts in the electrochemical CO2 reduction reaction, and summarizes research progress on synthesis methods, intrinsic activity differences of metal centers, and strategies for enhancing activity.
Review
Chemistry, Physical
Baohua Zhang, Yinzhu Jiang, Mingxia Gao, Tianyi Ma, Wenping Sun, Hongge Pan
Summary: This review summarized recent progress on hybrid electrocatalysts for efficient CO2RR, focusing on strategies for manipulating the metal-support interaction. Approaches for tuning metal-support interaction were discussed in detail from three aspects: metal active species, functional supports, and treatments of electrocatalysts.
Article
Chemistry, Applied
Zhiyan He, Xiaomei Ning, Guangxing Yang, Hongjuan Wang, Yonghai Cao, Feng Peng, Hao Yu
Summary: This article provides a comprehensive review of recent developments on glycerol selective oxidation over supported noble metal catalysts, with critical attention paid to the influence of metal-support and metal-metal interactions on the catalyst structure and performance, aiming for a better understanding of the reaction mechanism and rational catalyst design.
Review
Chemistry, Multidisciplinary
Jacob A. Barrett, Christopher J. Miller, Clifford P. Kubiak
Summary: The article reviews the research on electrocatalytic reduction of CO2 to CO using Group VII transition metal bipyridine catalysts over the past decade. Strategies to further advance our mechanistic understanding of the electrocatalytic reduction of CO2 to CO are described.
TRENDS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
Tiancheng Pu, Jiacheng Chen, Weifeng Tu, Jing Xu, Yi-Fan Han, Israel E. Wachs, Minghui Zhu
Summary: In this study, the strong metal-support interaction (SMSI) phenomenon for supported Ni/CeO2 catalysts with different CeO2 nanomorphologies was systematically explored. The degree of encapsulation of Ni particles originating from the SMSI effect was found to be positively correlated with the CO2 hydrogenation activity. Quasi in situ XPS and in situ DRIFTS techniques were used to reveal the relevant species and reaction pathways. These findings provide a fundamental strategy for tailoring catalytic performance by adjusting the support surface structure.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Chenghong Hu, Yajing Wang, Jianmin Chen, Hao-Fan Wang, Kui Shen, Kewen Tang, Liyu Chen, Yingwei Li
Summary: In this study, the authors demonstrate that introducing HER-inert main-group metal single atoms adjacent to transition-metal single atoms can enhance the CO2RR to CO without inducing the HER side reaction. The dual-metal Cu and In single-site atoms prepared by pyrolysis show superior catalytic performance compared to their monometallic counterparts.
Review
Chemistry, Multidisciplinary
Yasuomi Yamazaki, Masahiko Miyaji, Osamu Ishitani
Summary: This article summarizes the catalytic systems used for the reduction of low-concentration CO2, including the process of CO2 insertion into catalysts and the application of reaction media.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Engineering, Environmental
Malik Waqar Arshad, Young-Woo You, Young Jin Kim, Iljeong Heo, Seok Ki Kim
Summary: In this study, aluminum oxide (Al2O3) and titanium dioxide (TiO2)-supported iridium-ruthenium (IrRu) catalysts were synthesized and their catalytic performance in CO-assisted NO reduction was investigated. The results showed that IrRu bimetallic particles were well-alloyed on both supports, with TiO2 exhibiting a smaller size due to strong interactions with the metal. Interestingly, despite its larger particle size, IrRu/Al2O3 showed more efficient selective conversion of NOx to N2 compared to IrRu/TiO2. Mechanistic analysis suggested that the defect-free flat surface structure of the IrRu alloy contributed to its superior performance. The metal-support interfaces were found to be inactive regardless of their interaction strength.
CHEMICAL ENGINEERING JOURNAL
(2023)
Review
Chemistry, Physical
Fuping Pan, Xiaoxuan Yang, Thomas O'Carroll, Haoyang Li, Kai-Jie Chen, Gang Wu
Summary: This paper introduces the application of carbon materials in electrochemical CO2 reduction and proposes effective strategies to promote C2+ evolution. The relationship between the composition, structure, and morphology of carbon catalysts and their catalytic behavior is analyzed to establish catalytic mechanisms and critical factors. Future research directions and strategies are also discussed to inspire revolutionary advancements.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Wenying Zha, Diwen Liu, Zuju Ma, Yizhang Wang, Yiongcong Wei, Xiongfong Ma, Lele Wang, Qiqi Zhang, BenYong Lou, Rusheng Yuan, Xianzhi Fu, Rongjian Sa
Summary: This study investigated the electrocatalytic CO2 reduction reaction on monolayer C2N frameworks with metal clusters, showing that certain metal clusters can effectively catalyze CRR with lowered overpotentials.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Zhenhua Li, Jinjia Liu, Jiaqi Zhao, Run Shi, Geoffrey I. N. Waterhouse, Xiao-Dong Wen, Tierui Zhang
Summary: A novel L-Cu catalyst is successfully fabricated for photo-driven methanol steam reforming, which exhibits outstanding activity in hydrogen production. The L-Cu catalyst shows much higher hydrogen production rates under ultraviolet-visible irradiation compared to the dark condition at the same temperature. This study introduces a new photothermal strategy for hydrogen generation from methanol, demonstrating the enormous potential of photothermal catalysis in the chemical and energy sectors.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Xinyan Li, Shuhao Xiao, Dengji Guo, Jinxia Jiang, Xiaobin Niu, Rui Wu, Taisong Pan, Jun Song Chen
Summary: This study presents a template-free electrodeposition method for the growth of SbBi-Se self-supported nanowall arrays on copper substrates. The resulting heterostructured material exhibits uniformly dispersed phases and interfaces, which facilitate sodium ion diffusion and electronic conduction. The material demonstrates enhanced high-rate performance and superior cyclic retention, making it a promising candidate for sodium-ion battery applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Pu Wang, Run Shi, Yunxuan Zhao, Zhenhua Li, Jiaqing Zhao, Jiaqi Zhao, Geoffrey I. N. Waterhouse, Li-Zhu Wu, Tierui Zhang
Summary: In this study, the photocatalytic oxidative coupling of methane (OCM) over transition-metal-loaded ZnO photocatalysts was systematically investigated. A 1 wt% Au/ZnO catalyst exhibited remarkable C-2-C-4 hydrocarbon production rate and selectivity under light irradiation. The selectivity towards C-C coupling products strongly depends on the metal type and its interaction with ZnO. The findings suggest that the d-sigma center can be a suitable descriptor for predicting product selectivity during OCM over metal/ZnO photocatalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xuanang Bian, Yunxuan Zhao, Chao Zhou, Tierui Zhang
Summary: Enormous advances have been made in photothermal catalysis, but temperature assessment remains controversial in most photothermal catalytic systems. We revealed the phenomenon of temperature determination bias in gas-solid photothermal catalytic systems, which has been overlooked in most cases. To avoid temperature bias interference, we developed a universal protocol for reliable temperature evaluation by optimizing the reaction system. This study presents a functional and credible practice for temperature detection and emphasizes the effects of temperature differences in gas-solid photothermal catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xuanang Bian, Yunxuan Zhao, Geoffrey I. N. Waterhouse, Yingxuan Miao, Chao Zhou, Li-Zhu Wu, Tierui Zhang
Summary: This study measured the actual reaction temperature of photothermal ammonia synthesis over carbon-supported Ru catalyst using Le Chatelier's principle, and found that the activation energy for photothermal catalysis was much lower than thermocatalysis. This was attributed to hot-electron injection reducing the energy barriers for N2 dissociation and intermediates hydrogenation, while also suppressing carbon support methanation. The catalyst exhibited outstanding operational stability over 1000 hours. This work provides new insights into the effects of hot electrons in ammonia synthesis and guides the design of high-performance photothermal catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Yi Wang, Zhaohong Li, Xingqun Zheng, Rui Wu, Jianfeng Song, Yulin Chen, Xinzhe Cao, Yao Nie
Summary: Strong metal-support interaction (SMSI) plays an important role in tuning catalytic behavior by facilitating migration of reducible oxides from the support onto loaded metal surfaces and alloying of the guest metal with the metal component in the support. However, the conventional high-temperature redox treatment for SMSI is limited in achieving simultaneous occurrence of oxide migration and alloying mechanisms, which restricts its application in electrocatalysis. In this study, a low-temperature solvothermal-induced SMSI is established in the CeCuOx/C supported Pt system, leading to the partial encapsulation of supported Pt by CeOx and the alloying of Cu2+ in the substrate with guest Pt. This encapsulation and alloying processes significantly improve the catalysis configuration and restructure the geometric/electronic state of interfacial Pt atoms, resulting in enhanced performance for methanol oxidation reaction (MOR).
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Qi Zhou, Xueqiang Qi, Yiguang Zhou, Junyi Li, Jinxia Jiang, Hanchao Li, Xiaobin Niu, Rui Wu, Jun Song Chen
Summary: Lithium-selenium (Li-Se) batteries have attracted widely attention due to their high volume specific capacity and good electronic conductivity of selenium. However, the rapid capacity fading, high volume changes and shuttle effect of lithium polyselenides (LiPSes) limit its further application. In this study, a zinc-cobalt bimetallic catalysts on nitrogen-doped 3D ordered porous carbon (ZnCo-NC) was constructed and applied as cathode for Li-Se batteries, showing significantly improved performance compared to single-metal counterparts.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Materials Science, Multidisciplinary
Ding Zhang, Ellen Mitchell, Xunyu Lu, Dewei Chu, Lu Shang, Tierui Zhang, Rose Amal, Zhaojun Han
Summary: This review presents recent progress in different types of metal-free carbon-based catalysts for electrochemical production of H2O2. The fundamental aspects of the oxygen reduction reaction mechanism and performance evaluation are introduced. Catalysts with different dimensions, including 3D, 2D, 1D, and 0D, are reviewed. Strategies such as heteroatom doping, structural engineering, and defect engineering are examined for enhancing catalytic efficiency. Surface and interfacial engineering for high H2O2 production are discussed as well. Finally, challenges and opportunities in this field are proposed for the rational design of metal-free catalysts for electrochemical H2O2 production.
Article
Materials Science, Multidisciplinary
Si-Jia Zheng, Hua Cheng, Jin Yu, Qin Bie, Jing-Dong Chen, Feng Wang, Rui Wu, Daniel John Blackwood, Jun-Song Chen
Summary: A three-dimensional ordered porous nitrogen-doped carbon-supported Ni-N-x catalyst has been synthesized by direct pyrolysis of a mixture of SiO2, polyvinyl pyrrolidone, nickel-phenanthroline complex, followed by the removal of the SiO2 templates. The optimized catalyst exhibits a high CO Faradaic efficiency above 85% and a large CO current density of 16.2 mA.cm(-2), demonstrating superior CO2RR performance.
Article
Multidisciplinary Sciences
Jiaqi Zhao, Jinjia Liu, Zhenhua Li, Kaiwen Wang, Run Shi, Pu Wang, Qing Wang, Geoffrey I. N. Waterhouse, Xiaodong Wen, Tierui Zhang
Summary: The authors present a Ru1Co single atom alloy catalyst for CO photo-hydrogenation to C5+ liquid fuels. The catalyst demonstrates effective CO activation and C-C coupling reactions, while suppressing over-hydrogenation. The findings provide new opportunities for the production of C5+ liquid fuels under sunlight at mild pressures.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Chuang Fu, Xueqiang Qi, Lei Zhao, Tingting Yang, Qian Xue, Zhaozhao Zhu, Pei Xiong, Jinxia Jiang, Xuguang An, Haiyuan Chen, Jun Song Chen, Andreu Cabot, Rui Wu
Summary: A dual-atom catalyst, Zn/Fe-NC, is synthesized through pyrolysis of PVP coated on Fe-doped ZIF-8, and it shows outstanding activity for oxygen reduction reaction (ORR) with high half-wave potential, excellent stability, and resistance to methanol. Density functional theory calculation reveals that the ORR overpotential is only 0.282 V, and the down-shifted d band center of active Fe affected by Zn alleviates the adsorption of OH* intermediates, thus promoting the overall ORR electrocatalytic activity. Moreover, zinc-air batteries with Zn/Fe-NC catalyst as oxygen cathode demonstrate remarkable power density and specific capacity for practical applications.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Junyu Gao, Fan Wu, Yunxuan Zhao, Xuanang Bian, Chao Zhou, Junwang Tang, Tierui Zhang
Summary: Inspired by the enzyme nitrogenase, researchers have explored semiconductor photocatalytic nitrogen fixation because of its similar surface catalytic processes. In this study, a facile and efficient method was developed to regulate ZnO/ZnCr2O4 photocatalysts using ZnCr-layered double hydroxide (ZnCr-LDH) as precursors. By optimizing the composition ratio of Zn/Cr in ZnCr-LDH, enhanced nitrogen photofixation performance was achieved under ambient conditions. The improved photocatalytic activity was attributed to effective carrier separation efficiency due to the abundant composite interfaces. This work demonstrates a promising strategy for synthesizing nanocomposite photocatalysts for nitrogen photofixation and other challenging photocatalytic reactions.
Article
Multidisciplinary Sciences
Yingxuan Miao, Yunxuan Zhao, Geoffrey I. N. Waterhouse, Run Shi, Li-Zhu Wu, Tierui Zhang
Summary: Researchers have developed a photothermal catalytic recycling system that can convert polyolefin plastics into liquid/waxy fuels. By using concentrated sunlight or xenon lamp irradiation, polyolefin plastics are heated, resulting in the hydrogenolysis of the C-C and C-H bonds in the polymer chains, leading to the complete conversion of waste polyolefins into valuable liquid fuels. This work demonstrates a simple and efficient strategy for recycling waste polyolefin plastics using abundant solar energy.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Shuhao Xiao, Jinxia Jiang, Ying Zhu, Jing Zhang, Hanchao Li, Rui Wu, Xiaobin Niu, Jiaqian Qin, Jun Song Chen
Summary: FeSe2-xSx microspheres were prepared by self-doping solvothermal method and gas phase selenization. S doping improved the Na adsorption and lowered the diffusion energy barrier, enhancing the electronic conductivity of FeSe2-xSx. The carbon-free nature of the microspheres resulted in a low specific surface area and high tap density, leading to a high initial columbic efficiency. Compared with pure FeSe2, FeSe2-xSx exhibited a high reversible capacity and enhanced rate performance. Additionally, FeSe2-xSx//NVP pouch cells achieved high energy and volumetric energy densities, demonstrating the potential applications of FeSe2-xSx microspheres.
ADVANCED POWDER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zhao Li, Xueqiang Qi, Junjie Wang, Zhaozhao Zhu, Jinxia Jiang, Xiaobin Niu, Andreu Cabot, Jun Song Chen, Rui Wu
Summary: NiN4Cl-ClNC catalysts with atomically dispersed NiN4Cl active sites are prepared through a molten-salt-assisted pyrolysis strategy. The optimized catalyst shows excellent CO2 conversion activity and outstanding stability, delivering a high CO Faradaic efficiency of 98.7% and a remarkable CO partial current density of approximately 349.4 mA cm(-2) in flow-cell. The introduced axial Ni-Cl bond and ClC bond induce electronic delocalization, stabilizing Ni and facilitating the rate-determining step of COOH* formation.