Single Sb sites for efficient electrochemical CO2 reduction.

We report for the first time the facile synthesis of Sb single atoms supported on N-doped porous carbon. As compared to bulk Sb, Sb2O3, and Sb nanoparticles, that exhibit poor electrocatalytic CO2 reduction activity, the as-prepared Sb atomic sites enable efficient aqueous electroreduction of CO2 to CO with a high CO turnover frequency exceeding 16 500 h-1 at -0.9 V (versus the reversible hydrogen electrode), outperforming many other single atom electrocatalysts reported thus far.

Carbon-supported Ni nanoparticles for efficient CO2 electroreduction.

The development of highly selective, low cost, and energy-efficient electrocatalysts is crucial for CO2 electrocatalysis to mitigate energy shortages and to lower the global carbon footprint. Herein, we first report that carbon-coated Ni nanoparticles supported on N-doped carbon enable efficient electroreduction of CO2 to CO. In contrast to most previously reported Ni metal catalysts that resulted in severe hydrogen evolution during CO2 conversion, the Ni particle catalyst here presents an unprecedented CO faradaic efficiency of approximately 94% at an overpotential of 0.59 V, even comparable to that of the best single Ni sites. The catalyst also affords a high CO partial current density and a large CO turnover frequency, reaching 22.7 mA cm-2 and 697 h-1 at -1.1 V (versus the reversible hydrogen electrode), respectively. Experiments combined with density functional theory calculations showed that the carbon layer coated on Ni and N-dopants in carbon material both play important roles in improving catalytic activity for electrochemical CO2 reduction to CO by stabilizing *COOH without affecting the easy *CO desorption ability of the catalyst.

Heterogeneous electrochemical CO2 reduction using nonmetallic carbon-based catalysts: current status and future challenges.

Electrochemical CO2 reduction (ECR) offers an important pathway for renewable energy storage and fuels production. It still remains a challenge in designing highly selective, energy-efficient, robust, and cost-effective electrocatalysts to facilitate this kinetically slow process. Metal-free carbon-based materials have features of low cost, good electrical conductivity, renewability, diverse structure, and tunability in surface chemistry. In particular, surface functionalization of carbon materials, for example by doping with heteroatoms, enables access to unique active site architectures for CO2 adsorption and activation, leading to interesting catalytic performances in ECR. We aim to provide a comprehensive review of this category of metal-free catalysts for ECR, providing discussions and/or comparisons among different nonmetallic catalysts, and also possible origin of catalytic activity. Fundamentals and some future challenges are also described.