A wide range of CO : H2 syngas ratios enabled by a tellurization-induced amorphous telluride-palladium surface

被引:13
作者
Cao, Kailei [1 ]
Ji, Yujin [2 ]
Bai, Shuxing [1 ]
Huang, Xiaoqing [1 ,3 ]
Li, Youyong [2 ]
Shao, Qi [1 ]
机构
[1] Soochow Univ, Coll Chem Chem Engn & Mat Sci, Suzhou 215123, Jiangsu, Peoples R China
[2] Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Suzhou 215123, Jiangsu, Peoples R China
[3] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
基金
中国国家自然科学基金;
关键词
ELECTROCHEMICAL REDUCTION; ELECTROCATALYTIC REDUCTION; PD; ELECTROREDUCTION; CATALYSTS;
D O I
10.1039/d1ta04035a
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The direct production of syngas via the electrochemical CO2 reduction reaction (CO2RR) is a process with high potential due to its environmentally-friendliness and product adjustability properties. However, it is challenging to synthesize syngas with a wide range of tunable CO/H-2 ratios. Herein, we report that introducing tellurium (Te) can change the crystallinity of a palladium (Pd) surface, providing a unique amorphous surface to achieve a wide range of CO/H-2 ratios from 0.27 to 5.37. Compared with a highly crystalline Pd surface, the amorphous Te-Pd surface significantly increases the CO faradaic efficiency (FE), yet decreases the H-2 FE, leading to continuously tunable syngas. Detailed characterization shows that the surface tellurization of Pd nanoparticles (NPs) enhances the CO2 adsorption yet weakens the adsorption of COOH*, CO* and H* intermediates. Theoretical calculations further reveal that the amorphous Te-Pd surface shows a much lower barrier for the rate-determining step for CO* desorption, thus promoting CO generation. This work highlights the importance of the surface phase modification of metal electrocatalysts for the advanced CO2RR.
引用
收藏
页码:18349 / 18355
页数:7
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