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

Lin, X., Zhang, S.-N., Xu, D., Zhang, J.-J., Lin, Y.-X., Zhai, G.-Y., et al. (2021). Electrochemical activation of C–H by electron-deficient W2C nanocrystals for simultaneous alkoxylation and hydrogen evolution. Nature Communications, 12: 3882. doi:10.1038/s41467-021-24203-8.

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 Creators:
Lin, Xiu, Author
Zhang, Shi-Nan, Author
Xu, Dong, Author
Zhang, Jun-Jun, Author
Lin, Yun-Xiao, Author
Zhai, Guang-Yao, Author
Su, Hui, Author
Xue, Zhong-Hua, Author
Liu, Xi, Author
Antonietti, Markus1, Author           
Chen, Jie-Sheng, Author
Li, Xin-Hao, Author
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1Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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 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.

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Language(s): eng - English
 Dates: 2021-06-232021
 Publication Status: Issued
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 12 Sequence Number: 3882 Start / End Page: - Identifier: ISSN: 2041-1723

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Title: In Review
Source Genre: Journal
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Publ. Info: Research Square - Springer Nature
Pages: - Volume / Issue: - Sequence Number: 113168 Start / End Page: - Identifier: ISSN: 2693-5015