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液态金属制备二维非晶态SnO:大规模制备、相转移及电催化CO还原制甲酸

Two-Dimensional Amorphous SnO from Liquid Metal: Mass Production, Phase Transfer, and Electrocatalytic CO Reduction toward Formic Acid.

作者信息

Yuan Tingbiao, Hu Zheng, Zhao Yuxin, Fang Jinjie, Lv Jun, Zhang Qinghua, Zhuang Zhongbin, Gu Lin, Hu Shi

机构信息

Department of Chemistry, School of Science, Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Tianjin 300072, China.

School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.

出版信息

Nano Lett. 2020 Apr 8;20(4):2916-2922. doi: 10.1021/acs.nanolett.0c00844. Epub 2020 Mar 13.

DOI:10.1021/acs.nanolett.0c00844
PMID:32155077
Abstract

Liquid metal forms a thin layer of oxide skin via exposure to oxygen and this layer could be exfoliated by mechanical delamination or gas-injection/solvent-dispersion. Although the room-temperature fabrication of two-dimensional (2D) oxide through gas-injection and water-dispersion has been successfully demonstrated, a synthetic protocol in nonaqueous solvent at elevated temperature still remains as a challenge. Herein we report the mass-production of amorphous 2D SnO nanoflakes with Bi decoration from liquid Sn-Bi alloy and selected nonaqueous solvents. The functional groups of the solvents play a key role in determining the final morphology of the product and the hydroxyl-rich solvents exhibit the best control toward 2D SnO. The different solvent-oxide interaction that facilitates this phase-transfer process is further discussed on the basis of DFT calculation. Finally, the as-obtained 2D SnO is evaluated in electrocatalytic CO reduction with high faradaic efficiency (>90%) of formic acid and stable performance over 10 h.

摘要

液态金属通过暴露于氧气形成一层薄的氧化皮,这层氧化皮可通过机械分层或气体注入/溶剂分散来剥落。尽管通过气体注入和水分散在室温下制备二维(2D)氧化物已成功得到证明,但在高温非水溶剂中的合成方法仍然是一个挑战。在此,我们报告了从液态Sn-Bi合金和选定的非水溶剂大规模制备具有Bi修饰的非晶2D SnO纳米片。溶剂的官能团在决定产物的最终形态方面起着关键作用,富含羟基的溶剂对2D SnO表现出最佳的控制。基于密度泛函理论(DFT)计算,进一步讨论了促进这种相转移过程的不同溶剂-氧化物相互作用。最后,对所获得的2D SnO进行了电催化CO还原评估,其对甲酸的法拉第效率高(>90%)且在10小时内性能稳定。

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