Sui Rui, Pei Jiajing, Fang Jinjie, Zhang Xuejiang, Zhang Yufeng, Wei Feijun, Chen Wenxing, Hu Zheng, Hu Shi, Zhu Wei, Zhuang Zhongbin
State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China.
ACS Appl Mater Interfaces. 2021 Apr 21;13(15):17736-17744. doi: 10.1021/acsami.1c03638. Epub 2021 Apr 8.
The electrochemical CO reduction reaction (CORR) offers an environmentally benign pathway for renewable energy conversion and further regulation of the environmental CO concentration to achieve carbon cycling. However, developing desired electrocatalysts with high CO Faradaic efficiency (FE) at an ultralow overpotential remains a grand challenge. Herein, we report an effective CORR electrocatalyst that features Ag single-atom coordinated with three nitrogen atoms (Ag-N) anchored on porous concave N-doped carbon (Ag-N/PCNC), which is identified by X-ray absorption spectroscopy. Ag-N/PCNC shows a low CORR onset potential of -0.24 V, high maximum FE of 95% at -0.37 V, and high CO partial current density of 7.6 mA cm at -0.55 V, exceeding most of the previous Ag electrocatalysts. The in situ infrared absorption spectra technique proves that Ag-N single-atom sites have sole linear-adsorbed CO and can easily desorb *CO species to achieve the highest CO selectivity in comparison with the corresponding counterparts. This work provides significant inspiration on boosting CORR by tuning the active center at an atomic level to achieve a specific absorption with an intermediate.
电化学CO还原反应（CORR）为可再生能源转换以及进一步调节环境中CO浓度以实现碳循环提供了一条环境友好的途径。然而，开发在超低过电位下具有高CO法拉第效率（FE）的理想电催化剂仍然是一个巨大的挑战。在此，我们报道了一种有效的CORR电催化剂，其特征是Ag单原子与三个氮原子配位（Ag-N）锚定在多孔凹面N掺杂碳上（Ag-N/PCNC），这通过X射线吸收光谱法得以确定。Ag-N/PCNC显示出-0.24 V的低CORR起始电位、在-0.37 V时95%的高最大FE以及在-0.55 V时7.6 mA cm的高CO分电流密度，超过了大多数先前的Ag电催化剂。原位红外吸收光谱技术证明，与相应的对照物相比，Ag-N单原子位点具有唯一的线性吸附CO，并且能够轻松解吸*CO物种以实现最高的CO选择性。这项工作通过在原子水平上调节活性中心以实现与中间体的特定吸附，为促进CORR提供了重要的启发。
