Tian Zhihong, Zhang Qingran, Thomsen Lars, Gao Nana, Pan Jian, Daiyan Rahman, Yun Jimmy, Brandt Jessica, López-Salas Nieves, Lai Feili, Li Qiuye, Liu Tianxi, Amal Rose, Lu Xunyu, Antonietti Markus
Engineering Research Center for Nanomaterials, Henan University, Kaifeng, 475004, P. R. China.
Department of Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, 14476, Potsdam, Germany.
Angew Chem Int Ed Engl. 2022 Sep 12;61(37):e202206915. doi: 10.1002/anie.202206915. Epub 2022 Aug 8.
The electrochemical oxygen reduction reaction (ORR) provides a green route for decentralized H O synthesis, where a structure-selectivity relationship is pivotal for the control of a highly selective and active two-electron pathway. Here, we report the fabrication of a boron and nitrogen co-doped turbostratic carbon catalyst with tunable B-N-C configurations (CNB-ZIL) by the assistance of a zwitterionic liquid (ZIL) for electrochemical hydrogen peroxide production. Combined spectroscopic analysis reveals a fine tailored B-N moiety in CNB-ZIL, where interfacial B-N species in a homogeneous distribution tend to segregate into hexagonal boron nitride domains at higher pyrolysis temperatures. Based on the experimental observations, a correlation between the interfacial B-N moieties and HO selectivity is established. The CNB-ZIL electrocatalysts with optimal interfacial B-N moieties exhibit a high HO selectivity with small overpotentials in alkaline media, giving a HO yield of ≈1787 mmol g h at -1.4 V in a flow-cell reactor.
电化学氧还原反应（ORR）为分散式过氧化氢合成提供了一条绿色途径，其中结构-选择性关系对于控制高选择性和活性的双电子途径至关重要。在此，我们报道了通过两性离子液体（ZIL）辅助制备具有可调B-N-C构型（CNB-ZIL）的硼氮共掺杂乱层碳催化剂用于电化学过氧化氢生产。结合光谱分析揭示了CNB-ZIL中精细定制的B-N部分，其中均匀分布的界面B-N物种在较高热解温度下倾向于聚集成六方氮化硼域。基于实验观察结果，建立了界面B-N部分与H₂O₂选择性之间的相关性。具有最佳界面B-N部分的CNB-ZIL电催化剂在碱性介质中表现出高H₂O₂选择性和小过电位，在流动池反应器中于-1.4 V时H₂O₂产率约为1787 mmol g⁻¹ h⁻¹ 。
