Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H2 Production

Yanmin Hu; Tingting Chao; Yapeng Li; Peigen Liu; Tonghui Zhao; Ge Yu; Cai Chen; Xiao Liang; Huile Jin; Shuwen Niu; Wei Chen; Dingsheng Wang; Yadong Li

doi:10.1002/anie.202308800

Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H₂ Production

Angew Chem Int Ed Engl. 2023 Aug 28;62(35):e202308800. doi: 10.1002/anie.202308800. Epub 2023 Jul 20.

Authors

Yanmin Hu^{1

2}, Tingting Chao^{1

2}, Yapeng Li¹, Peigen Liu², Tonghui Zhao¹, Ge Yu², Cai Chen², Xiao Liang³, Huile Jin¹, Shuwen Niu^{1

2}, Wei Chen¹, Dingsheng Wang³, Yadong Li³

Affiliations

¹ Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, China.
² Center of Advanced Nanocatalysis (CAN), Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, China.
³ Department of Chemistry, Tsinghua University, Beijing, China.

PMID: 37428114
DOI: 10.1002/anie.202308800

Abstract

Water electrolysis for H₂ production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru₁ -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of -60 mV and overpotential of 32 mV for a current density of 10 mA cm^-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall hydrazine splitting (OHzS) demonstrates outstanding activity with a record-high current density of 522 mA cm^-2 at cell voltage of 0.3 V. DFT calculations elucidate the cooperative Ni(Co)-Ru-P sites in Ru₁ -NiCoP optimize H* adsorption, and enhance adsorption of *N₂ H₂ to significantly lower the energy barrier for hydrazine dehydrogenation. Moreover, a self-powered H₂ production system utilizing OHzS device driven by direct hydrazine fuel cell (DHzFC) achieve a satisfactory rate of 24.0 mol h^-1 m^-2 .

Keywords: Dehydrogenation; Hydrazine Oxidation Reaction; Interfacial Sites; Overall Hydrazine Splitting; Single-Atom Catalyst.

Grants and funding

22171157/National Natural Science Foundation of China