Electrochemical activation of C–H by electron-deficient W2C nanocrystals for simultaneous alkoxylation and hydrogen evolution

Xiu Lin, Shi-Nan Zhang, Dong Xu, Jun-Jun Zhang, Yun-Xiao Lin, Guang-Yao Zhai, Hui Su, Zhong-Hua Xue, Xi Liu, Markus Antonietti, Jie-Sheng Chen and Xin-Hao Li ()
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Xiu Lin: Shanghai Jiao Tong University
Shi-Nan Zhang: Shanghai Jiao Tong University
Dong Xu: Shanghai Jiao Tong University
Jun-Jun Zhang: Shanghai Jiao Tong University
Yun-Xiao Lin: Shanghai Jiao Tong University
Guang-Yao Zhai: Shanghai Jiao Tong University
Hui Su: Shanghai Jiao Tong University
Zhong-Hua Xue: Shanghai Jiao Tong University
Xi Liu: Shanghai Jiao Tong University
Markus Antonietti: Max-Planck Institute of Colloids and Interfaces, Wissenschaftspark Golm
Jie-Sheng Chen: Shanghai Jiao Tong University
Xin-Hao Li: Shanghai Jiao Tong University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract The activation of C–H bonds is a central challenge in organic chemistry and usually a key step for the retro-synthesis of functional natural products due to the high chemical stability of C–H bonds. Electrochemical methods are a powerful alternative for C–H activation, but this approach usually requires high overpotential and homogeneous mediators. Here, we design electron-deficient W2C nanocrystal-based electrodes to boost the heterogeneous activation of C–H bonds under mild conditions via an additive-free, purely heterogeneous electrocatalytic strategy. The electron density of W2C nanocrystals is tuned by constructing Schottky heterojunctions with nitrogen-doped carbon support to facilitate the preadsorption and activation of benzylic C–H bonds of ethylbenzene on the W2C surface, enabling a high turnover frequency (18.8 h−1) at a comparably low work potential (2 V versus SCE). The pronounced electron deficiency of the W2C nanocatalysts substantially facilitates the direct deprotonation process to ensure electrode durability without self-oxidation. The efficient oxidation process also boosts the balancing hydrogen production from as-formed protons on the cathode by a factor of 10 compared to an inert reference electrode. The whole process meets the requirements of atomic economy and electric energy utilization in terms of sustainable chemical synthesis.

Date: 2021
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DOI: 10.1038/s41467-021-24203-8

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