Sub-2 nm ultra-thin Bi2O2CO3 nanosheets with abundant Bi-O structures toward formic acid electrosynthesis over a wide potential window
Sub-2 nm ultra-thin Bi2O2CO3 nanosheets with abundant Bi-O structures toward formic acid electrosynthesis over a wide potential window
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DOI：
10.1007/s12274-021-3903-0
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发表时间：
2021-10
期刊：
影响因子：
9.9
通讯作者：
Yuhong Wang;Bin Wang;Wenjun Jiang;Zailun Liu;Jiangwei Zhang;Li-Zhen Gao;Wei‐Jing Yao
中科院分区：
文献类型：
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作者：
Yuhong Wang;Bin Wang;Wenjun Jiang;Zailun Liu;Jiangwei Zhang;Li-Zhen Gao;Wei‐Jing Yao
电催化还原CO2制甲酸（ERC-HCOOH）是缓解能源危机和解决环境问题的最可行途径之一。然而，ERC-HCOOH在宽的潜在窗口中保持优异的活性和选择性仍然是一个挑战。本文通过拓扑变换和后处理在碳纸上原位合成了具有丰富Bi-O结构的超薄花状Bi 2 O2 CO 3纳米片（NS）。HCOOH（FEHCOOH）的法拉第效率在宽电位窗口（−1.5至−1.8 V vs. Ag/AgCl）内达到90%。值得注意的是，在-1.8 V vs. Ag/AgCl下实现了优异的FEHCOOH（90%）和电流密度（47 mA·cm−2）。X射线吸收精细结构（XAFS）结合密度泛函理论（DFT）计算表明，Bi 2 O2 CO 3 NS的优异性能归因于其丰富的Bi-O结构，有利于增强CO2* 和OCHO* 中间体的吸附，并能有效抑制析氢。Bi_2O_2CO_3NS在较宽电位窗口内的优异性能为CO_2的高效电催化转化提供了新的思路。
The electrocatalytic reduction of CO2to HCOOH (ERC-HCOOH) is one of the most feasible ways to alleviate energy crisis and solve environmental problems. Nevertheless, it remains a challenge for ERC-HCOOH to maintain excellent activity and selectivity in a wide potential window. Herein, ultra-thin flower-like Bi2O2CO3nanosheets (NSs) with abundant Bi-O structures werein situsynthesized on carbon paper via topological transformation and post-processing. Faraday efficiency of HCOOH (FEHCOOH) reached 90% in a wide potential window (−1.5 to −1.8 V vs. Ag/AgCl). Significantly, excellent FEHCOOH(90%) and current density (47 mA·cm−2) were achieved at −1.8 V vs. Ag/AgCl. The X-ray absorption fine structure (XAFS) combined with density functional theory (DFT) calculation demonstrated that the excellent performance of Bi2O2CO3NS was attributed to the abundant Bi-O structures, which was conducive to enhancing the adsorption of CO2* and OCHO* intermediates and can effectively inhibit hydrogen evolution. The excellent performance of Bi2O2CO3NS over a wide potential window could provide new insights for the efficient electrocatalytic conversion of CO2.