Nano Energy ( IF 16.8 ) Pub Date : 2023-06-25 , DOI: 10.1016/j.nanoen.2023.108638
Xiao-Du Liang , Qi-Zheng Zheng , Nian Wei , Yao-Yin Lou , Sheng-Nan Hu , Kuang-Min Zhao , Hong-Gang Liao , Na Tian , Zhi-You Zhou , Shi-Gang Sun
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Bi-based electrocatalysts are prominent candidates to achieve CO2 reduction to formate with high selectivity but suffer from unsatisfied activity, stability, and ambiguous nature of active sites. Herein, the Bi@Bi2O2CO3 nanosheet catalyst is designed via an electrochemical in-situ reconstruction approach from BiPO4. The conversion processes were revealed by electrochemical in-situ Raman and FTIR spectroscopy. The obtained Bi@Bi2O2CO3 catalyst demonstrates high CO2 reduction performance (FEHCOOH ≈ 100%, jHCOOH ≈ −60 mA cm−2) and excellent stability of 110 h in H-type cell. Moreover, the Bi@Bi2O2CO3 delivers a remarkable formate partial current density up to −1.2 A cm−2 (production rate as 22.4 mmol cm−2 h−1) in the flow cell. DFT theoretical studies reveal the synergistic effect of Bi and Bi2O2CO3 at the interface played an important role in changing the adsorption behavior of reaction intermediates and further greatly reducing the activation barrier of the conversion of *OCHO to *HCOOH during CO2 reduction.
中文翻译:
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原位构建Bi@Bi2O2CO3纳米片催化剂用于安培级CO2电还原生成甲酸盐
双基电催化剂是实现高选择性将CO 2还原为甲酸盐的重要候选者,但其活性、稳定性和活性位点的性质不明确,但其活性、稳定性不令人满意。在此,Bi@Bi 2 O 2 CO 3纳米片催化剂是通过BiPO 4的电化学原位重构方法设计的。通过电化学原位拉曼光谱和 FTIR 光谱揭示了转化过程。所得Bi@Bi 2 O 2 CO 3催化剂表现出较高的CO 2还原性能(FE HCOOH ≈ 100%, jHCOOH ≈ -60 mA cm -2 ),在 H 型电池中具有 110 小时的优异稳定性。此外,Bi@Bi 2 O 2 CO 3在流通池中提供高达-1.2 A cm -2的显着甲酸盐部分电流密度(生产率为22.4 mmol cm -2 h -1 )。DFT理论研究揭示了Bi和Bi 2 O 2 CO 3在界面处的协同效应对于改变反应中间体的吸附行为发挥了重要作用,并进一步大大降低了CO 2过程中*OCHO转化为*HCOOH的活化势垒减少。