Journal ArticleDOI
Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction.
Xinyue Wang,Yu Wang,Xiahan Sang,Wanzhen Zheng,Shihan Zhang,Ling Shuai,Bin Yang,Zhongjian Li,Jianmeng Chen,Lecheng Lei,Nadia Mohd Adli,Michael K.H. Leung,Ming Qiu,Gang Wu,Yang Hou +14 more
TLDR
Theoretical calculations elucidate that the introduction of axial oxygen atom could optimize surface states of Ni-N4 moieties and enhance the charge polarization effect, therefore decreasing the potential barrier of intermediate COOH* formation, a key factor to accelerate the reaction kinetics and boost the CO2RR performance.Abstract:
Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4 ) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2 RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4 -O/C). The Ni-N4 -O/C electrocatalyst exhibited excellent CO2 RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at -0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from -0.5 to -1.1 V. The superior CO2 RR activity is due to the Ni-N4 -O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.read more
Citations
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Journal ArticleDOI
Advances and Challenges for the Electrochemical Reduction of CO2 to CO: From Fundamentals to Industrialization
TL;DR: In this paper, the authors give an overview of recent advances and challenges for the selective conversion of CO2 into CO. Multidimensional catalyst and electrolyte engineering for the CO2 RR are also summarized.
Journal ArticleDOI
A Supported Pd 2 Dual‐Atom Site Catalyst for Efficient Electrochemical CO 2 Reduction
Ningqiang Zhang,Xinxin Zhang,Yikun Kang,Chenliang Ye,Rui Jin,Han Yan,Rui Lin,Jiarui Yang,Qian Xu,Yu Wang,Qinghua Zhang,Lin Gu,Licheng Liu,Weiyu Song,Jian Liu,Dingsheng Wang,Yadong Li +16 more
TL;DR: The density functional theory (DFT) calculations revealed that the intrinsic reason for the superior activity of Pd 2 DAC toward CO 2 RR was the electron transfer between Pd atoms at the dimeric Pd sites, which was beneficial for CO production in CO 2RR.
Journal ArticleDOI
Proton Capture Strategy for Enhancing Electrochemical CO2 Reduction on Atomically Dispersed Metal-Nitrogen Active Sites*.
Xinyue Wang,Xiahan Sang,Chung-Li Dong,Siyu Yao,Ling Shuai,Jianguo Lu,Bin Yang,Zhongjian Li,Lecheng Lei,Ming Qiu,Liming Dai,Yang Hou +11 more
TL;DR: In this article, a proton capture strategy was developed by accelerating the water dissociation reaction catalyzed by transition-metal nanoparticles (NPs) adjacent to atomically dispersed and nitrogen-coordinated single nickel (Ni-Nx ) active sites to accelerate proton transfer to the latter for boosting the intermediate protonation step, and thus the whole ECR process.
Journal ArticleDOI
Engineering Single-Atomic Ni-N4-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting.
Xiaomeng Zhang,Panlong Zhai,Yanxue Zhang,Yunzhen Wu,Chen Wang,Lei Ran,Junfeng Gao,Zhuwei Li,Bo Zhang,Zhaozhong Fan,Licheng Sun,Licheng Sun,Jungang Hou +12 more
TL;DR: In this paper, a versatile coupling strategy was developed to engineer atomically dispersed Ni-N4 sites coordinated with an axial direction oxygen atom (NiN4-O) incorporated between oxygen evolution cocatalyst (OEC) and semiconductor photoanode, boosting the photogenerated electron-hole separation and thus improving PEC activity.
Journal ArticleDOI
Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction.
Ke Li,Sheng Han Zhang,Xiuli Zhang,Shuang Liu,Haiyan Jiang,Taoli Jiang,Chunyue Shen,Yi Yu,Wei Chen +8 more
TL;DR: In this paper , a single-Fe-atom catalyst with phosphorus (Fe-N/P-C) was used for CO2 reduction in commercial carbon black as a robust electrocatalyst.
References
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Journal ArticleDOI
Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications
TL;DR: In this article, the authors highlight and summarize recent advances in wet-chemistry synthetic methods for single-atom catalysts with special emphasis on how to achieve the stabilization of single metal atoms against migration and agglomeration.
Journal ArticleDOI
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
Hongbin Yang,Hongbin Yang,Sung Fu Hung,Song Liu,Song Liu,Kaidi Yuan,Shu Miao,Liping Zhang,Xiang Huang,Hsin-Yi Wang,Weizheng Cai,Rong Chen,Jiajian Gao,Xiaofeng Yang,Wei Chen,Yanqiang Huang,Hao Ming Chen,Chang Ming Li,Tao Zhang,Bin Liu +19 more
TL;DR: In this paper, the atomically dispersed nickel on nitrogenated graphene was identified as an efficient and durable electrocatalyst for CO2 reduction based on operando X-ray absorption and photo-electron spectroscopy measurements, and the monovalent Ni(i) atomic center with a d9 electronic configuration is identified as the catalytically active site.
Journal ArticleDOI
Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells
Jiazhan Li,Jiazhan Li,Mengjie Chen,David A. Cullen,Sooyeon Hwang,Maoyu Wang,Boyang Li,Kexi Liu,Stavros Karakalos,Marcos Lucero,Hanguang Zhang,Chao Lei,Hui Xu,George E. Sterbinsky,Zhenxing Feng,Dong Su,Karren L. More,Guofeng Wang,Zhen-Bo Wang,Gang Wu +19 more
TL;DR: In this article, Wu et al. reported an efficient oxygen reduction reaction (ORR) catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C).
Journal ArticleDOI
Exclusive Ni-N4 Sites Realize Near-Unity CO Selectivity for Electrochemical CO2 Reduction.
Xiaogang Li,Wentuan Bi,Minglong Chen,Yuexiang Sun,Huanxin Ju,Wensheng Yan,Junfa Zhu,Xiaojun Wu,Wangsheng Chu,Changzheng Wu,Yi Xie +10 more
TL;DR: Topo-chemical transformation by carbon layer coating successfully ensures preservation of the Ni-N4 structure to a maximum extent and avoids the agglomeration of Ni atoms to particles, providing abundant active sites for the catalytic reaction.
Journal ArticleDOI
Edge-Site Engineering of Atomically Dispersed Fe-N4 by Selective C-N Bond Cleavage for Enhanced Oxygen Reduction Reaction Activities.
TL;DR: Both experiments and theoretical calculations verified the selective C-N bond cleavage adjacent to Fe center induced by porosity engineering could form edge-hosted Fe-N4 moieties, and therefore lower the overall oxygen reduction reaction barriers comparing to intact atomic configuration.