Article
Materials Science, Multidisciplinary
Long Lin, Kun Xie, Linghao Zhu, Chaozheng He, Zhanying Zhang
Summary: In this study, a novel high-efficiency electrocatalyst Rh-BC3N2 was constructed and simulated using first-principles calculations to reveal the mechanism behind the enhanced electrocatalytic reduction of CO2. The results show that Rh atom can be stably supported on top of N site of BC3N2 monolayer. The research provides a promising candidate for CO2 reutilization and valuable insights for future practical design.
MATERIALS TODAY COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Zhiming Wei, Yuhang Liu, Jie Ding, Qinye He, Qiao Zhang, Yueming Zhai
Summary: Sulfur-doped cobalt-nitrogen-carbon single-atom catalyst (Co1-SNC) exhibits superior performance in the electrocatalytic CO2 reduction reaction (CO2RR) compared to the sulfur-free counterpart (Co1-NC). In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), kinetic isotope effect (KIE), and theoretical calculation demonstrate that sulfur doping can promote water activation, elevate the d-band center of Co active site, and reduce the free energy of *COOH intermediate formation. This work deepens the understanding of heteroatom-doped single-atom catalysts in designing efficient CO2RR processes.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Energy & Fuels
Beibei An, Guanyao Yu, Jinya Li, Yuanyuan Li, Li Wang, Jinglai Zhang
Summary: Electrocatalysis of CO2 reduction reaction has great potential for application but faces challenges due to the inertness of CO2 and hydrogen evolution reaction. By developing robust catalysts, screening transition metals, and regulating N-doping amount, the catalytic activity can be improved.
Article
Chemistry, Physical
Chongyang Li, Cui Shang, Bin Zhao, Gang Zhang, Liangliang Liu, Wentao Yang, Zhiquan Chen
Summary: The effect of a bimetallic dimer-embedded anatase TiO2(101) surface on CO2 reduction behaviors was explored using first-principles calculations. The results showed that Zn-Cu dimer could stably stay on the TiO2 surface and promote the adsorption and reduction of CO2. In terms of barrier energy and activity, Zn-Cu dimer might be a more suitable and economical choice.
Article
Materials Science, Multidisciplinary
Jin-Hang Liu, Xiaohua Cao, Ruirui Wang, Xiudong Chen, Yawei Wang, Pinghua Yang, Jiamin Long, Xiaojie Yin, Zijian Huang, Dapeng Cao
Summary: In this study, a series of TM-N2O2Cx (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) single-atom catalysts were designed and their catalytic activities for CO2RR were investigated using density functional theory. The results showed that these catalysts exhibited excellent selectivity towards three different CO2RR products, including CH4, CO, and HCOOH at relatively low overpotentials. The CO2RR products of Sc-N2O2Cx, Mn-N2O2Cx, and Zn-N2O2Cx were CO, while V-N2O2Cx produced CH4, and the other six catalysts produced HCOOH. Moreover, the best pathway for CH4 formation was also revealed. These TM-N2O2Cx catalysts demonstrated high catalytic activity for electrocatalytic CO2RR, providing useful information for the synthesis of promising CO2RR catalysts by experimental scientists.
SCIENCE CHINA-MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yucheng Cao, Suya Chen, Shuowen Bo, Wenjun Fan, Jiangnan Li, Chunmei Jia, Zhen Zhou, Qinghua Liu, Lirong Zheng, Fuxiang Zhang
Summary: This study reports a single-atom bismuth-decorated copper alloy catalyst that can effectively modulate the selectivity of carbon dioxide reduction to multi-carbon products. The catalyst exhibits superior performance and stability, making it a promising candidate for electrocatalytic reduction of CO2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Haoran Guo, Pengfei Yuan, Jun Zhao, Jiayang Zhao, Qian Peng, Rui Song
Summary: By modulating the orbital electronic state of the active site, solar-driven CO2 reduction into hydrocarbons can promote CO2 utilization and address environmental issues. Our study finds that MoSi2N4 decorated with single atoms of 3d and 4d transition metals can serve as efficient photocatalysts for CO2 reduction, and the selectivity of the products is correlated with the d-band center of the transition metals. Additionally, introducing strain can improve catalytic performance.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Ling-Chan Tian, Jin-Nian Hu, Yang Meng, Jin-Xia Liang, Chun Zhu, Jun Li
Summary: In this study, a non-noble metal catalyst, nickel single-atom catalyst (SAC) of Ni-1/UiO-66-NH2, was reported for the electrochemical reduction of CO2 to CH4. The catalyst exhibited high stability and selectivity, with CH4 being the predominant product. Theoretical calculations showed that the Ni-1/UiO-66-NH2 catalyst had a low limiting potential and suppressed the competitive hydrogen evolution reaction. This work provides a theoretical foundation for the further development and application of SAC electrocatalysts in CO2 reduction.
Article
Chemistry, Physical
Gurpreet Kour, Xin Mao, Aijun Du
Summary: The electrochemical reduction of carbon dioxide to generate value-added chemicals or fuels using renewable energy resources is a promising approach to mitigate greenhouse gases. Developing highly efficient catalysts with minimum energy input and maximum conversion efficiency is a critical challenge. Mononuclear and dinuclear complexes of Cr, Mn, Fe, Co and Ni with macrocyclic Schiff-base calixpyrrole ligands were studied for catalyzing the reduction of CO2 to methane or methanol. Iron-containing mononuclear complex showed the highest activity and selectivity for transforming CO2 to CH4 with a very low negative limiting potential of -0.24 V, offering a technique for developing electrocatalysts with great potential for CO2 reduction reactions.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Yixin Wang, Ming Zheng, Xin Wang, Xin Zhou
Summary: By performing density functional theory (DFT) calculations, it is found that Zn-based single atom alloys (SAAs) are promising electrocatalysts for the reduction of CO2 to C-1 hydrocarbons. The study screens stable alloys and discusses their reaction mechanisms. The computational results suggest that Zn-based SAAs can reduce CO2 to methane with a small overpotential.
Article
Chemistry, Multidisciplinary
Dawei Xi, Jiayi Li, Jingxiang Low, Keke Mao, Ran Long, Jiawei Li, Zehui Dai, Tianyi Shao, Yuan Zhong, Yu Li, Zibiao Li, Xian Jun Loh, Li Song, Enyi Ye, Yujie Xiong
Summary: Carbon-supported Ni single-atom catalysts with precisely controlled single-atom structure achieved through joule heating strategy show superior performance in electrocatalytic carbon dioxide reduction reaction, with 80% of N dopants coordinated with metal elements, thereby avoiding unfavorable N species and demonstrating unprecedented activity, selectivity, and stability.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Neng Li, Xiao Wang, Xuelian Lu, Peng Zhang, Wee-Jun Ong
Summary: A series of non-noble metal single-atom catalysts of Mo2CS2-MXene for CO2 reduction have been systematically investigated, with Fe-Mo2CS2 showing the lowest limiting potential and highest electrocatalytic activity. These catalysts can effectively inhibit the competitive hydrogen evolution reaction and control the products of CO2 reduction to be non-completely CH4. Ab initio molecular dynamics simulations have also demonstrated the stable existence of these catalysts at room temperature, highlighting their promising potential for electrochemical reduction of CO2.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Engineering, Environmental
Shuai Liu, Mengmeng Jin, Jiaqiang Sun, Yongji Qin, Sanshuang Gao, Yu Chen, Shusheng Zhang, Jun Luo, Xijun Liu
Summary: In this study, Fe-SA/BNC material was successfully fabricated and exhibited excellent CO2 reduction reaction activity, achieving remarkable current density and Faradaic efficiency through MEA. Density functional theory (DFT) calculations revealed the positive effect of introducing B on the desorption of *CO. Furthermore, the assembled Zn-CO2 battery demonstrated outstanding peak power density and stability for CO production.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Jiazhi Wang, Qi Hao, Haixia Zhong, Kai Li, Xinbo Zhang
Summary: In this study, an isolated single-atom Ni catalyst regulated strategy was developed to activate and stabilize the iron phthalocyanine molecule (Ni SA@FePc) for a highly efficient CO2RR process at low overpotential. Ni SA@FePc showed significantly enhanced CO2RR performance compared to single-atom Ni catalyst and FePc molecule, thanks to its well-defined and homogenous catalytic centers with unique structures.
Article
Chemistry, Physical
Liu Guo, Rui Li, Jiawei Jiang, Ji-Jun Zou, Wenbo Mi
Summary: Single-atom catalysts with magnetic elements have been widely utilized as efficient OER electrocatalysts. By investigating the adsorption of different contents of transition metal atom Mn on g-C3N4, it was found that 2Mn-C3N4 exhibited higher OER activity and lower over-potential compared to Mn-C3N4. The metal-support interaction can influence the OER performance, with orbital hybridization intensity playing an important role in the catalytic activity.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)