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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
2D Borophene Oxide Substrate for C2+ Products Synthesis via CO2 Electroreduction at Industrial Current Densities
Peng Chen1, Yuhang Wang2, Haojian Lin3
1Department of Mechanical Engineering, The University of Hong Kong, Pokfulam, Hong Kong, China.
Abstract:
The industrialization of electrochemical CO2 reduction reaction for multi-carbon products synthesis is limited by HER competition, sluggish C─C coupling kinetics, and carbonate deposition. Through rational computational screening, we identify β-rhombohedral borophene oxide (β-rh. BO) as an ideal two-dimensional substrate to simultaneously overcome these bottlenecks. Evaluated in a flow cell with 1 M KOH electrolyte, the β-rh. BO-supported Cu (BO-Cu) demonstrates outstanding performance across an industrially relevant current density range of -700 to -1500 mA cm-2, achieving a peak C2+ Faradaic efficiency (FE) of 85.9% and a partial current density exceeding -1082 mA cm-2. Mechanistic studies reveal that β-rh. BO serves a role beyond an electron donor. Specifically, it redistributes hydrated K+ and alters the interfacial water structure, which not only suppresses HER by diverting proton transfer toward *CO hydrogenation rather than H2 evolution, but also enables the transformation of symmetric C─C coupling to asymmetric C─C coupling via modulating the charge distribution of intermediates. Furthermore, the introduction of β-rh. BO drastically reduces carbonate deposition. This work presents a novel multifunctional substrate that synergistically modulates the electronic structure, tailors interfacial water structure, and suppresses carbonate deposition, offering a new paradigm for the design of electrocatalysts for industrial CO2RR applications.
