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间隙 Sn 掺杂促进铋电催化 CO2 转化为甲酸盐,Science China Materials

间隙 Sn 掺杂促进铋电催化 CO2 转化为甲酸盐

Science China Materials

(

IF

7.4

)

Pub Date : 2023-07-20

, DOI:

10.1007/s40843-023-2495-7

Xin Xu, Yang Wei, Linhua Mi, Guodong Pan, Yajun He, Siting Cai, Chaoyang Zheng, Yaming Jiang, Bin Chen, Liuyi Li, Shenghong Zhong, Jianfeng Huang, Wenbin Hu, Yan Yu

电化学CO 2还原（CO 2 RR）是一项很有前途的技术，可以减轻温室效应并将CO 2转化为增值化学品。然而，实现目标产物的高催化活性、选择性和稳定性仍然是一个巨大的挑战。本文中，间隙Sn掺杂Bi（Sn x -Bi，x是Sn与Bi的原子比，x =1/2、1/16、1/24或1/40）纳米线束（NB）通过还原来制备Sn掺杂的Bi 2 S 3。值得注意的是，Sn 1/24 -Bi NB 在 1400 mV 的宽电位窗口内表现出超高的甲酸选择性（-0.5 至 -1.9 V 的法拉第效率超过 90% ）可逆氢电极（RHE）），在-1.9 V vs. RHE下具有-319 mA cm -2的工业兼容电流密度。此外，在~−200 mA cm -2下实现了超过84小时的优异长期稳定性。实验结果和密度泛函理论（DFT）计算表明，间隙掺杂Sn优化了*OCHO中间体的吸附亲和力，降低了铋催化剂的电子转移能垒，从而产生了显着的CO 2 RR性能。这项研究为设计具有增强的电化学CO 2转化为甲酸盐的催化活性、选择性和耐久性的掺杂电催化剂提供了宝贵的灵感。

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Interstitial Sn-doping promotes electrocatalytic CO2-to-formate conversion on bismuth

Electrochemical CO2 reduction (CO2RR) is a promising technology to mitigate the greenhouse effect and convert CO2 to value-added chemicals. Yet, achieving high catalytic activity, selectivity, and stability for target products is still a big challenge. Herein, interstitially Sn-doped Bi (Snx-Bi, x is the atomic ratio of Sn to Bi, x = 1/2, 1/16, 1/24 or 1/40) nanowire bundles (NBs) are prepared by reducing Sn-doped Bi2S3. Notably, Sn1/24-Bi NBs exhibit ultrahigh formate selectivity over a broad potential window of 1400 mV (Faradaic efficiency over 90% from −0.5 to −1.9 V vs. reversible hydrogen electrode (RHE)) with an industry-compatible current density of −319 mA cm−2 at −1.9 V vs. RHE. Moreover, superior long-term stability for more than 84 h at ∼−200 mA cm−2 is realized. Experimental results and density functional theory (DFT) calculations reveal that interstitially doped Sn optimizes the adsorption affinity of *OCHO intermediate and reduces the electron transfer energy barrier of bismuth catalyst, resulting in the remarkable CO2RR performance. This study provides valuable inspiration for the design of doped electrocatalysts with enhanced catalytic activity, selectivity, and durability for electrochemical CO2-to-formate conversion.

更新日期：2023-07-20