Qian Qizhu, Zhang Jihua, Li Jianming, Li Yapeng, Jin Xu, Zhu Yin, Liu Yi, Li Ziyun, El-Harairy Ahmed, Xiao Chong, Zhang Genqiang, Xie Yi
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Guizhou Education University, Guiyang, Guizhou, 550018, P. R. China.
Angew Chem Int Ed Engl. 2021 Mar 8;60(11):5984-5993. doi: 10.1002/anie.202014362. Epub 2021 Jan 27.
Electrochemical water splitting for H production is limited by the sluggish anode oxygen evolution reaction (OER), thus using hydrazine oxidation reaction (HzOR) to replace OER has received great attention. Here we report the hierarchical porous nanosheet arrays with abundant Ni N-Co N heterointerfaces on Ni foam with superior hydrogen evolution reaction (HER) and HzOR activity, realizing working potentials of -43 and -88 mV for 10 mA cm , respectively, and achieving an industry-level 1000 mA cm at 200 mV for HzOR. The two-electrode overall hydrazine splitting (OHzS) electrolyzer requires the cell voltages of 0.071 and 0.76 V for 10 and 400 mA cm , respectively. The H production powered by a direct hydrazine fuel cell (DHzFC) and a commercial solar cell are investigated to inspire future practical applications. DFT calculations decipher that heterointerfaces simultaneously optimize the hydrogen adsorption free energy (ΔG ) and promote the hydrazine dehydrogenation kinetics. This work provides a rationale for advanced bifunctional electrocatalysts, and propels the practical energy-saving H generation techniques.
用于制氢的电化学水分解受到阳极析氧反应（OER）缓慢的限制，因此使用肼氧化反应（HzOR）来替代OER受到了广泛关注。在此，我们报道了在泡沫镍上具有丰富Ni-N-Co-N异质界面的分级多孔纳米片阵列，其具有优异的析氢反应（HER）和HzOR活性，在10 mA cm⁻²时的工作电位分别为-43和-88 mV，并且在200 mV时实现了HzOR的1000 mA cm⁻²的工业级电流密度。两电极全肼分解（OHzS）电解槽在10和400 mA cm⁻²时分别需要0.071和0.76 V的电池电压。研究了由直接肼燃料电池（DHzFC）和商用太阳能电池驱动的制氢过程，以启发未来的实际应用。密度泛函理论（DFT）计算表明，异质界面同时优化了氢吸附自由能（ΔG）并促进了肼脱氢动力学。这项工作为先进的双功能电催化剂提供了理论依据，并推动了实际节能制氢技术的发展。
