Surface Immobilization of Transition Metal Ions on Nitrogen‐Doped Graphene Realizing High‐Efficient and Selective CO₂ Reduction

Abstract

Electrochemical conversion of CO to value-added chemicals using renewable electricity provides a promising way to mitigate both global warming and the energy crisis. Here, a facile ion-adsorption strategy is reported to construct highly active graphene-based catalysts for CO reduction to CO. The isolated transition metal cyclam-like moieties formed upon ion adsorption are found to contribute to the observed improvements. Free from the conventional harsh pyrolysis and acid-leaching procedures, this solution-chemistry strategy is easy to scale up and of general applicability, thus paving a rational avenue for the design of high-efficiency catalysts for CO reduction and beyond.

Nitrogen‐Doped Graphene Quantum Dots Enhance the Activity of Bi2O3 Nanosheets for Electrochemical Reduction of CO2 in a Wide Negative Potential Region

“…ForB i 2 O 3 -NGQDs simulation, we adopted ah eterojunction model composed of single-layer Bi 2 O 3 and NGQDs.T he whole reaction pathway for electrochemical reduction CO 2 to HCOOH is at wo-electron and two-proton transfer process through the OCHO* intermediate and adsorbed HCOOH-(ads). [22] Bi 2 O 3 -NGQDs demonstrates am ore positive DP limit of 1.33 Vt han that of Bi 2 O 3 (À0.35 V; Figure S15), which coincides exactly with the higher formate selectivity observed in experimental results. Both Bi 2 O 3 -NGQDs and Bi 2 O 3 show al argest energy barrier (DG)f or OCHO* formation, demonstrating the initial proton-coupled electron transfer is the potential limiting step,w hich is in good agreement with the result of Tafel analysis.E ncouragingly, after combining with NGQDs,the DG for OCHO* formation decreases from 1.41 eV for Bi 2 O 3 to 0.66 eV for Bi 2 O 3 -NGQDs,whereas the energy barrier for the competitive HER raised from 1.06 eV for Bi 2 O 3 to 1.99 eV for Bi 2 O 3 -NGQDs ( Figure S14).…”

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

“…d) Schematic illustration of Ni SACs based on an impregnation–adsorption method. Reproduced with permission . Copyright 2018, Wiley‐VCH.…”

Optimizing Electron Densities of Ni‐N‐C Complexes by Hybrid Coordination for Efficient Electrocatalytic CO2 Reduction

“…In particular, metal‐supported N‐doped carbon (M‐N‐C) composites have shown excellent activity and selectivity for CO production from CO 2 RR . In these M‐N‐C structures, the M‐N 4 (typically Ni‐N 4 ) center is usually proposed to be the possible active site . However, under high‐temperature synthesis conditions of the M‐N‐C catalysts, the resulting materials are likely to form complex structures, such as M‐N x ( x= 1–4), M‐C x , and defects in the carbon matrix, which makes identifying the real active site difficult .…”