Synergistic Cu-Co Sites Enabled Reversible H₂ Storage and Release in Liquid Organic Hydrogen Carriers.

Authors

Qingju Wang, Kevin M Siniard, Yuanpeng Zhang, Murillo L Martins, Yongqiang Cheng, Alexander S Ivanov, Jorge Anibal Boscoboinik, Esteban Luis Fornero, Gerd Duscher, Shuai Yuan, De-En Jiang, Nikolaos Samartzis, Nabihan B Abdul Rahman, Felipe Polo-Garzon, Zhenzhen Yang, Sheng Dai

Published in

Angewandte Chemie (International ed. in English). Nov 11, 2026. Epub Nov 11, 2026.

Abstract

Liquid organic hydrogen carriers (LOHCs) offer a practical platform for reversible hydrogen storage, a critical bottleneck in the global transition to clean energy. However, their reliance on noble-metal catalysts and separate catalysts for hydrogenation and dehydrogenation cycles remains a major barrier to practical deployment. Here, we report an earth-abundant, heterostructured ternary oxide catalyst (CuCoCeO_x) that enables efficient, reversible, and bidirectional hydrogenation-dehydrogenation of LOHCs such as carbazoles over multiple cycles without any pretreatment. Driven by the in situ reaction-induced reconstruction, the catalyst dynamically evolves and stabilizes functionally decoupled Cu(δ⁺)-CoO_x interfacial sites, where the defective, amorphous CoO_x nanodomains anchor bulky LOHC substrates, complementing adjacent Cu sites for reversible hydrogen shuttling. Detailed characterizations and comparison with CuCeO_x and CoCeO_x reveal the indispensable synergy between coexisting Cu and Co sites. Reduced Cu species facilitate the generation of low-valence Co sites, while Co species suppress the over-reduction and sintering of Cu, collectively stabilizing abundant Cu(δ⁺)-CoO_x interfacial sites as the catalytically active centers. This dynamic structural reconstruction delivers 98.4% H₂ uptake and near-quantitative H₂ release, with stable performance over five consecutive LOHC cycles, substantially surpassing commercial noble-metal benchmarks.

PMID:
43012482
Bibliographic data and abstract were imported from PubMed on 11 Nov 2026.

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