Chang Jiuli, Hu Zhanqiang, Wu Dapeng, Xu Fang, Chen Chen, Jiang Kai, Gao Zhiyong
School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Xinxiang, Henan 453007, PR China.
Key Laboratory of Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, Henan Key Laboratory for Environment Pollution Control, International Joint Laboratory on Key Techniques in Water Treatment, Henan Province, School of Environment, Henan Normal University, Xinxiang, Henan 453007, PR China.
J Colloid Interface Sci. 2023 May 15;638:801-812. doi: 10.1016/j.jcis.2023.02.037. Epub 2023 Feb 11.
Efficient and bifunctional nonprecious catalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are essential for the production of green hydrogen via water electrolysis. Transition metal (Ni, Co, Fe, etc.) phosphides are frequently documented HER catalysts, whereas their bimetallic oxides are efficient OER catalysts, thus enabling bifunctional catalysis for water electrolysis via proper operation. Herein, phosphide-reduced graphene oxide (rGO) hybrids were prepared from graphene oxide (GO)-incorporated bimetal Prussian blue analog (PBA) precursors. The hybrids could experience partial surface oxidation to create oxide layers with OER activities, and the hybrids also possessed considerable HER properties, therefore enabling bifunctional catalytic features for water electrolysis. The typical NiFeP-rGO hybrid demonstrated an overpotential of 250 mV at 10 mA cm and good durability for OER, as well as moderate HER catalytic features (overpotential of 165 mV at -10 mA cm and acceptable catalytic stability). Due to the bifunctional catalytic features, the NiFeP-rGO-based symmetric water electrolyzer demonstrated a moderate input voltage and high faradaic efficiency (FE) for O and H production. The current work provides a feasible way to prepare OER and HER bifunctional catalysts by facile phosphorization of PBA-associated precursors and spontaneous surface oxidation. Given the oxidation/reduction bifunctional catalytic behaviors, phosphide-rGO hybrid catalysts have great potential for widespread application in fields beyond water electrolysis, such as electrochemical pollution abatement, sensors, energy devices and organic syntheses.
用于析氧反应(OER)和析氢反应(HER)的高效双功能非贵金属催化剂对于通过水电解生产绿色氢气至关重要。过渡金属(镍、钴、铁等)磷化物是经常被报道的HER催化剂,而它们的双金属氧化物是高效的OER催化剂,因此通过适当操作能够实现水电解的双功能催化。在此,磷化物还原氧化石墨烯(rGO)杂化物由掺入氧化石墨烯(GO)的双金属普鲁士蓝类似物(PBA)前驱体制备而成。这些杂化物可经历部分表面氧化以形成具有OER活性的氧化层,并且杂化物还具有可观的HER性能,因此实现了水电解的双功能催化特性。典型的NiFeP-rGO杂化物在10 mA cm时的过电位为250 mV,具有良好的OER耐久性,以及适度的HER催化特性(在-10 mA cm时过电位为165 mV,催化稳定性可接受)。由于具有双功能催化特性,基于NiFeP-rGO的对称水电解槽在产生氧气和氢气时表现出适度的输入电压和高法拉第效率(FE)。当前工作提供了一种通过对PBA相关前驱体进行简便磷化和自发表面氧化来制备OER和HER双功能催化剂的可行方法。鉴于其氧化/还原双功能催化行为,磷化物-rGO杂化催化剂在水电解以外的领域,如电化学污染治理、传感器、能量装置和有机合成等方面具有广泛应用的巨大潜力。