Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas,Small

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Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas
Small ( IF 13.0 ) Pub Date : 2023-04-07 , DOI: 10.1002/smll.202300417
Fangqi Yang _{1,

2} , Caihong Liang ₃ , Weizhen Zhou ₁ , Wendi Zhao ₄ , Pengfei Li _{5,

6} , Zhengyu Hua ₁ , Haoming Yu ₁ , Shixia Chen ₁ , Shuguang Deng ₇ , Jing Li ₈ , Yeng Ming Lam _{3,

9} , Jun Wang ₁

Affiliation

School of Chemistry and Chemical Engineering, Nanchang University, No. 999 Xuefu Avenue, Jiangxi, 330031, China.
School of Materials Science and Engineering, Nanjing University of Posts and Telecommunications, No. 9 Wenyuan Road, Nanjing, 210023, China.
School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798.
School of Resources and Environment, Nanchang University, No. 999 Xuefu Avenue, Jiangxi, 330031, China.
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou, 350207, China.
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543.
School for Engineering of Matter, Transport and Energy, Arizona State University, 551 E. Tyler Mall, Tempe, AZ, 85287, USA.
School of Chemistry, Beihang University, Beijing, 100191, China.
Facility for Analysis, Characterisation, Testing and Simulation (FACTS), Nanyang Technological University, Singapore, 639798.

Post-combustion flue gas (mainly containing 5–40% CO₂ balanced by N₂) accounts for about 60% global CO₂ emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a β-Bi₂O₃-derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO₂, N_2, and flue gas. During pure CO₂ electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH₃) FE of 18.53% and yield rate of 11.5 µg h⁻¹ mg_cat⁻¹ in pure N₂ atmosphere. Noticeably, in simulated flue gas (15% CO₂ balanced by N₂ with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO₂ and N₂ molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.

中文翻译：

氧化物铋作为电化学还原烟气的高效催化剂

燃烧后烟气（主要含有5%~40%的CO ₂，平衡为N ₂）约占全球CO ₂排放量的60%。将烟气合理转化为增值化学品仍然是一个艰巨的挑战。在此，这项工作报道了一种具有表面配位氧的β-Bi ₂ O ₃衍生的铋（OD-Bi）催化剂，用于纯CO ₂、N ₂和烟道气的有效电还原。纯CO ₂电还原过程中，甲酸盐的最大法拉第效率(FE)达到98.0%，并且在600 mV的宽电位下保持在90%以上，长期稳定50 h。此外，OD-Bi在纯N ₂气氛中实现了18.53%的氨(NH _{3 ) FE和11.5 µg h}^-1 mg _cat^-1的产率。值得注意的是，在模拟烟气中（15% CO ₂由带有微量杂质的 N ₂平衡），流通池内的最大甲酸盐 FE 为 97.3%，同时在 700 mV 的宽电位范围内获得了 90% 以上的甲酸盐 FE 。原位拉曼结合理论计算表明，OD-Bi中的表面配位氧物种可以通过选择性地分别有利于*OCHO和*NNH中间体的吸附来显着活化CO ₂和N _2分子。这项工作提供了一种表面氧调节策略，以开发高效的铋基电催化剂，以直接将商业相关的烟气转化为有价值的化学品。

更新日期：2023-04-07

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