Stable and Efficient Single-Atom Zn Catalyst for CO₂ Reduction to CH₄

Abstract

The development of highly active and durable catalysts for electrochemical reduction of CO2 (ERC) to CH4 in aqueous media is an efficient and environmentally friendly solution to address global problems in energy and sustainability. In this work, an electrocatalyst consisting of single Zn atoms supported on microporous N-doped carbon was designed to enable multielectron transfer for catalyzing ERC to CH4 in 1 M KHCO3 solution. This catalyst exhibits a high Faradaic efficiency (FE) of 85%, a partial current density of −31.8 mA cm–2 at a potential of −1.8 V versus saturated calomel electrode, and remarkable stability, with neither an obvious current drop nor large FE fluctuation observed during 35 h of ERC, indicating a far superior performance than that of dominant Cu-based catalysts for ERC to CH4. Theoretical calculations reveal that single Zn atoms largely block CO generation and instead facilitate the production of CH4.

Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

“…3b) and CO 2 -to-CH 4 conversion rate of 0.17 μmol cm −2 s −1 of CoO-2.5 nm/Cu/PTFE, which improve by a factor of 2.6x relative to the best previous reports having a CH 4 FE higher than 50% (Supplementary Table 2). The catalyst system reported herein achieved a half-cell energy efficiency of 27% in neutral medium (Supplementary Note 1), which is among the best previously reported catalysts with current densities above 50 mA cm −2 (Supplementary Table 2) [13][14][15][16][17][18][19][20] . We then tested the stability of the CoO-2.5 nm/Cu/PTFE catalyst system.…”

“…This motivates the need for practical electrolyzers which convert CO 2 to CH 4 at high rates and energy efficiency 9,10 . Along the way to this goal, further progress is required in the electrocatalysts which facilitate the conversion chemistry [11][12][13][14][15][16][17][18][19][20] . By judicious adjustment of CO 2 partial pressure, copper (Cu) catalysts have attained a 48% faradaic efficiency (FE) to CH 4 (ref.…”

Metal‐Free Multi‐Heteroatom‐Doped Carbon Bifunctional Electrocatalysts Derived from a Covalent Triazine Polymer

“…The ever-increasing energy demand promotes the vigorous exploitation of advanced and green energy techniques, such as rechargeable metal-air batteries, fuel cells, water electrolysis technologies, etc. [1][2][3][4][5][6][7][8][9] However, the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) during discharge and charge processes has severely hampered their widespread applications. [10,11] Efficient electrocatalysts are required to accelerate ORR and OER.…”

Advances in Metal Phthalocyanine based Carbon Composites for Electrocatalytic CO2 Reduction

“…Nowadays, the reduction of carbon dioxide into hydrocarbons or carbon oxides through secondary energy. Such as carbon monoxide, ethylene, methanol, formic acid, methane, ethanol [14][15][16][17][18][19] etc.. In turn, value-added chemicals and fuels can be used further to avoid dependence on fossil fuels and reduce annual carbon emissions.…”