Interfacial Electron Engineering of PdSn‐NbN/C for Highly Efficient Cleavage of the C–C Bonds in Alkaline Ethanol Electrooxidation

Author:

Ye Na1,Sheng Wenchao2,Zhang Riguang3,Yan Binhang4,Jiang Zhao1ORCID,Fang Tao1

Affiliation:

1. Department of Chemical Engineering Shaanxi Key Laboratory of Energy Chemical Process Intensification Engineering Research Center of New Energy System Engineering and Equipment Xi'an Jiaotong University Xi'an 710049 China

2. College of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai 200092 China

3. State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of Technology Taiyuan 030000 China

4. Department of Chemical Engineering Tsinghua University Beijing 100084 China

Abstract

AbstractThe splitting of the C–C bonds of ethanol remains a key issue to be addressed, despite tremendous efforts made over the past several decades. This study highlights the enhancement mechanism of inexpensive NbN‐modified Pd1Sn3‐NbN/C towards the C–C bonds cleavage for alkaline ethanol oxidation reaction (EOR). The optimal Pd1Sn3‐NbN/C delivers a catalytic activity up to 43.5 times higher than that of commercial Pd/C and high carbonate selectivity (20.5%) toward alkaline EOR. Most impressively, the Pd1Sn3‐NbN/C presents good durability even after 25 200 s of chronoamperometric testing. The enhanced catalytic performance is mainly due to the interfacial interaction between PdSn and NbN, demonstrated by multiple structural characterization results. In addition, in situ ATR‐SEIRAS (Attenuated total reflection‐surface enhanced infrared absorption spectroscopy) results suggest that NbN facilitates the C–C bonds cleavage towards the alkaline EOR, followed by the enhanced OH adsorption to promote the subsequent oxidation of C1 intermediates after doping Sn. DFT (density functional theory) calculations indicate that the activation barriers of the C–H bond cleavage in CH3CH2OH, CH3CHOH, CH3CHO, CH3CO, CH2CO, and the C–C bond cleavage in CH3CO, CH2CO, CHCO are evidently reduced and the removal of adsorbed CH3CO and CO becomes easier on the PdSn‐NbN/C catalyst surface.

Funder

National Natural Science Foundation of China

Taiyuan University of Technology

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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