Journal ArticleDOI
Identification of Single-Atom Ni Site Active toward Electrochemical CO2 Conversion to CO.
Haesol Kim,Dongyup Shin,Woojin Yang,Da Hye Won,Hyung Suk Oh,Min Wook Chung,Donghyuk Jeong,Sun Hee Kim,Keun Hwa Chae,Ji Yeon Ryu,Junseong Lee,Sung June Cho,Jiwon Seo,Hyungjun Kim,Chang Hyuck Choi +14 more
TLDR
In this article, the authors investigated CO2 electrolysis of Ni sites with well-defined coordination, tetraphenylporphyrin (N4-TPP) and 21-oxatetrameryl porphrin (N3O-TPP), and found that the broken ligand-field symmetry is the key for active CO 2 electrolysis.Abstract:
Electrocatalytic conversion of CO2 into value-added products offers a new paradigm for a sustainable carbon economy. For active CO2 electrolysis, the single-atom Ni catalyst has been proposed as promising from experiments, but an idealized Ni-N4 site shows an unfavorable energetics from theory, leading to many debates on the chemical nature responsible for high activity. To resolve this conundrum, here we investigated CO2 electrolysis of Ni sites with well-defined coordination, tetraphenylporphyrin (N4-TPP) and 21-oxatetraphenylporphyrin (N3O-TPP). Advanced spectroscopic and computational studies revealed that the broken ligand-field symmetry is the key for active CO2 electrolysis, which subordinates an increase in the Ni redox potential yielding NiI. Along with their importance in activity, ligand-field symmetry and strength are directly related to the stability of the Ni center. This suggests the next quest for an activity-stability map in the domain of ligand-field strength, toward a rational ligand-field engineering of single-atom Ni catalysts for efficient CO2 electrolysis.read more
Citations
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Posted ContentDOI
Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries
Xiao Hai,Shibo Xi,Sharon Mitchell,Karim Harrath,Karim Harrath,Haomin Xu,Dario Faust Akl,Debin Kong,Jing Li,Zejun Li,Tao Sun,Huimin Yang,Yige Cui,Chenliang Su,Xiaoxu Zhao,Jun Li,Jun Li,Javier Pérez-Ramírez,Jiong Lu +18 more
TL;DR: In this paper, a general approach combining wet-chemistry impregnation and two-step annealing is devised for the scalable synthesis of a library of ultra-high-density single-atom catalysts with drastically enhanced reactivity.
Journal ArticleDOI
Structure Sensitivity in Single-Atom Catalysis toward CO2 Electroreduction
TL;DR: Owing to unique electronic structure and high atom utilization, single-atom catalysts (SACs) have displayed unprecedented activity and selectivity toward a wide range of catalytic reactions.
Unified mechanistic understanding of CO2 reduction to CO on transition metal and single atom catalysts
TL;DR: In this article, a unified mechanistic picture of CO2 reduction to CO on transition metal and single atom catalysts is presented, including the decisive CO2* and COOH* binding strengths.
Journal ArticleDOI
Optimizing the Electrocatalytic Selectivity of Carbon Dioxide Reduction Reaction by Regulating the Electronic Structure of Single‐Atom M‐N‐C Materials
TL;DR: In this article , the authors systematically summarize effective means, including reasonable selection of isolated metal sites, regulation of the coordination environment, and fabrication of dimetallic single-atom sites for attaining optimal geometric and electronic structures of M−N−C materials and further correlate these structures with catalytic selectivity to various C1 and C2 products in the CO2RR.
Journal ArticleDOI
Integrating Single Atoms with Different Microenvironments into One Porous Organic Polymer for Efficient Photocatalytic CO 2 Reduction.
TL;DR: In this article, a series of porous organic polymers is designed and prepared simultaneously, containing well-defined M-N4 and m-N2 O2 single-atom sites.
References
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Noémie Elgrishi,Kelley J. Rountree,Brian D. McCarthy,Eric S. Rountree,Thomas T. Eisenhart,Jillian L. Dempsey +5 more
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Journal ArticleDOI
On the preparation of metalloporphyrins
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
Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis
Ming Gong,Wu Zhou,Mon-Che Tsai,Jigang Zhou,Mingyun Guan,Meng-Chang Lin,Bo Zhang,Yongfeng Hu,Di Yan Wang,Jiang Yang,Stephen J. Pennycook,Bing-Joe Hwang,Hongjie Dai +12 more
TL;DR: N nanoscale nickel oxide/nickel heterostructures formed on carbon nanotube sidewalls as highly effective electrocatalysts for hydrogen evolution reaction with activity similar to platinum are reported.
Journal ArticleDOI
Catalysis of the electrochemical reduction of carbon dioxide
TL;DR: The general trends that transpire presently and are likely to be the object of active future work emphasis is put on the favorable role of acid addition in homogeneous catalytic systems and on the crucial chemical role of the electrode material in heterogeneous catalysis.