期刊
SEPARATION AND PURIFICATION TECHNOLOGY
卷 289, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.seppur.2022.120731
关键词
Electrocatalytic hydrodechlorination; Electronic structure; Pd-Au alloy; Mass activity; Electron-rich
资金
- Chongqing Science and Technology Commission [cstc2019jscx-gksbX0032]
- Chongqing Education Commission [KJZD-K201800801, KJZD-M201900802]
- Taishan Scholars Program of Shandong Province [tsqn201909065]
- Shandong Provincial Natural Science Foundation [ZR2021YQ15, ZR2020QB174]
- National Natural Science Foundation of China [22108306]
The electronic structure of Pd catalyst has been regulated by designing bimetallic Pd-Au alloy nanoparticles with electron-rich Pd, which greatly improves the efficiency of electrocatalytic hydrodechlorination. Experimental characterization and theoretical calculation show that electron-rich Pd promotes the desorption of dechlorination products and accelerates the renewal of active sites. This work provides a strategy for electronic structure engineering of Pd-based electrocatalysts, opening a new opportunity for the design of high-performance hydrodechlorination catalysts.
Regulating the electronic structure of Pd catalyst for promoting electrocatalytic hydrodechlorination is promising but still challenging. Herein, we propose an electronic structure engineering for accelerating the hydrodechlorination process by desigining bimetallic Pd-Au alloy nanoparticles (ANs) with electron-rich Pd as high efficiency electrocatalysts. The Pd7Au3 ANs exhibits the highest electrocatalytic hydrodechlorination activity, the 4-chlorophenol hydrodechlorination efficiency reaches 98.35 % within 4 h, and the mass activity is 0.47 h(-1) mgPd(-1), which is 7.83 times as high as that of pure Pd nanoparticles. The experimental characterization and theoretical calculation reveal that Pd atoms obtain electrons and gold atoms lose electrons in Pd-Au ANs, resulting in the formation of electron-rich Pd, which promotes the desorption of the dechlorination product phenol and accelerates the renewal of active sites. This work provides an electronic structure engineering strategy of Pd-based electrocatalysts for electrocatalytic hydrodechlorination, which opens a new opportunity for rational design and construction of high-performance hydrodechlorination catalysts.
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