Tuning the local electronic structure of a single-site Ni catalyst by co-doping a 3D graphene framework with B/N atoms toward enhanced CO₂ electroreduction

Abstract

Various single metal sites supported on N-doped carbon materials have been demonstrated to be the effective catalysts for CO2 electroreduction. However, it remains a challenging task to gain comprehensive understanding...

Ni single atoms supported on hierarchically porous carbonized wood with highly active Ni–N4sites as a self-supported electrode for superior CO2electroreduction

“…3f ). 26 Furthermore, as revealed by the EXAFS wavelet transform (WT) analysis and the resulting WT contour plots, in contrast to the intensity maximum that arises from the Ni-Ni bond at 7.18 Å −1 for Ni foil and the Ni-O bond at 4.46 Å −1 for NiO, only one intensity maximum at 3.66 Å −1 is found for Ni SAs-NCW, which is very close to that of NiPc (3.95 Å −1 ), which further confirms the Ni-N 4 coordination.…”

Microenvironment Modulation in Carbon‐Supported Single‐Atom Catalysts for Efficient Electrocatalytic CO2 Reduction

“…Additionally, Xiong et al . reported that, with the coordination of B in the higher coordination shell, the performance of Ni SACs can be enhanced [71] . Particularly, the catalyst named Ni−B 2 N 4 delivered the highest Faradaic efficiency of CO with 98% at the overpotential of −0.8 V, because the B‐doping changed the electronic structure of Ni and reduced the energy barrier of generating COOH*.…”

Single-site catalysts for CO2 electroreduction

“…In recent decades, single-site catalysts (SSCs) have emerged as a new type of catalyst because of their precisely controllable structure and high atomic utilization efficiency. [9][10][11][12][13][14][15][16] The SSCs with active metal center isolated by non-metal atoms mainly contain single-atom catalysts (SACs), 17,18 homogeneous molecular catalysts (HMCs), 19,20 as well as metal organic framework-supported (MOF-supported) 21,22 and covalent organic framework-supported (COF-supported) SSCs. 23,24 The unique coordination environment of SSCs paves a new way for regulating the intrinsic charge, spinning order, and charge transfer of catalysts.…”

“…In addition, the controllable structure of SSCs is also beneficial for the structural design of catalyst, study of reaction mechanism, and evolution of reaction products during the ECR reaction. 14,25–27 Numerous theoretical and experimental studies have demonstrated the application potential of SSCs in ECR. 28–31…”

“…In addition, the controllable structure of SSCs is also beneficial for the structural design of catalyst, study of reaction mechanism, and evolution of reaction products during the ECR reaction. 14,[25][26][27] Numerous theoretical and experimental studies have demonstrated the application potential of SSCs in ECR. [28][29][30][31] In this review, we comprehensively summarize the researches on these emerging SSCs for ECR, including their catalytic mechanisms, synthesis, optimization strategies, and remaining challenges.…”