Atomically Dispersed Cobalt/Copper Dual-Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Yanzhe Shi, Bingcheng Luo, Runqi Liu, Rui Sang, Dandan Cui, Henrik Junge, Yi Du, Tianle Zhu, Matthias Beller, Xiang Li

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

The development of practical materials for (de)hydrogenation reactions is a prerequisite for the launch of a sustainable hydrogen economy. Herein, we present the design and construction of an atomically dispersed dual-metal site Co/Cu−N−C catalyst allowing significantly improved dehydrogenation of formic acid, which is available from carbon dioxide and green hydrogen. The active catalyst centers consist of specific CoCuN6 moieties with double-N-bridged adjacent metal-N4 clusters decorated on a nitrogen-doped carbon support. At optimal conditions the dehydrogenation performance of the nanostructured material (mass activity 77.7 L ⋅ gmetal−1 ⋅ h−1) is up to 40 times higher compared to commercial 5 % Pd/C. In situ spectroscopic and kinetic isotope effect experiments indicate that Co/Cu−N−C promoted formic acid dehydrogenation follows the so-called formate pathway with the C−H dissociation of HCOO* as the rate-determining step. Theoretical calculations reveal that Cu in the CoCuN6 moiety synergistically contributes to the adsorption of intermediate HCOO* and raises the d-band center of Co to favor HCOO* activation and thereby lower the reaction energy barrier.

Original languageEnglish
Article numbere202313099
JournalAngewandte Chemie International Edition in English
Volume62
Issue number43
DOIs
StatePublished - 23 Oct 2023
Externally publishedYes

Keywords

  • Bimetallic Materials
  • Cobalt and Copper.
  • Dehydrogenation Catalysis
  • Dual Metal Sites
  • Formic Acid

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