Amorphous N_xC Coating Promotes Electrochemical CO₂ Deep Reduction to Hydrocarbons over Ag Nanocatalysts

TY - JOUR

T1 - Amorphous NxC Coating Promotes Electrochemical CO2 Deep Reduction to Hydrocarbons over Ag Nanocatalysts

AU - Cui, Yanjia

AU - Yang, Caili

AU - Lin, Huanhao

AU - Rui, Suyan

AU - Yao, Defu

AU - Liao, Yuting

AU - Zhang, Chenchen

AU - Fang, Yiwen

AU - Wang, Xiaoming

AU - Zhong, Ziyi

AU - Song, Yibing

AU - Wang, Gongwei

AU - Zhuang, Lin

AU - Li, Zhen

PY - 2022/12/13

Y1 - 2022/12/13

N2 - The electrochemical conversion of CO2 into high value-added hydrocarbon products provides a promising path to reduce the dependence on fossil energy and close carbon cycle. Cu-based catalyst is so far the only material that can effectively realize this process, limiting the optional catalysts for industrial application. Therefore, it is urgent to design other strategies to boost hydrocarbon products beyond Cu-based materials. Here, the NxC shell is constructed on the surface of Ag nanoparticle core (core-shell structure Ag@NxC) to boost the formation of CH4 and CH2CH2. The NxC shell does not modify the electronic property of Ag but prolongs the residence time of the CO intermediate to enhance the C-C coupling and deep reduction, which are proved by in situ ATR-SEIRAS. In addition, the activated H2O molecules could provide sufficient adsorbed H to enhance the further reduction of the carbonaceous intermediate during the CO2 reduction reaction. As a result, the Faradaic efficiency (FE) of the hydrogen evolution reaction is enhanced over the Ag@NxC-2 catalyst (∼12% at-1.4 V vs RHE), and the FEs of CH4 and CH2CH2 are significantly enhanced (above 43.8 and 8.4%, respectively). Our findings provide a strategy to achieve the conversion of CO2 into hydrocarbon products over non-Cu-based catalysts.

AB - The electrochemical conversion of CO2 into high value-added hydrocarbon products provides a promising path to reduce the dependence on fossil energy and close carbon cycle. Cu-based catalyst is so far the only material that can effectively realize this process, limiting the optional catalysts for industrial application. Therefore, it is urgent to design other strategies to boost hydrocarbon products beyond Cu-based materials. Here, the NxC shell is constructed on the surface of Ag nanoparticle core (core-shell structure Ag@NxC) to boost the formation of CH4 and CH2CH2. The NxC shell does not modify the electronic property of Ag but prolongs the residence time of the CO intermediate to enhance the C-C coupling and deep reduction, which are proved by in situ ATR-SEIRAS. In addition, the activated H2O molecules could provide sufficient adsorbed H to enhance the further reduction of the carbonaceous intermediate during the CO2 reduction reaction. As a result, the Faradaic efficiency (FE) of the hydrogen evolution reaction is enhanced over the Ag@NxC-2 catalyst (∼12% at-1.4 V vs RHE), and the FEs of CH4 and CH2CH2 are significantly enhanced (above 43.8 and 8.4%, respectively). Our findings provide a strategy to achieve the conversion of CO2 into hydrocarbon products over non-Cu-based catalysts.

U2 - 10.1021/acscatal.2c04580

DO - 10.1021/acscatal.2c04580

M3 - 文章

SN - 2155-5435

SP - 169

EP - 178

JO - ACS Catalysis

JF - ACS Catalysis

ER -