Mingjie Sun , Simiao Sha , Riyue Ge , Bin Liu , Qingqiao Fu , Wenxian Li
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引用次数: 0
Abstract
The rational design of bifunctional heterostructured catalysts for overall water splitting, which enhance electron transfer and mass exchange at the catalyst-electrolyte interface, is crucial for advancing green hydrogen production. Herein, CoP/Mo4P3 heterojunctions with hierarchical (macro-meso-micro) porous structures are designed to induce intense electron coupling at the interface of CoP and Mo4P3 and enhance catalytic stability, mass exchange efficiency as well as active species utilization for total hydrolysis. The growth of CoP/Mo4P3 within hierarchically porous nitrogen-doped carbon polyhedra occurs via cation exchange between Mo ions and glycerite-etched hollow ZIF-67, followed by pyrolysis and phosphidation. The CoP/Mo4P3 heterointerface interaction enables remodeled electronic structure and increased active sites, improving H2O dissociation capacity and intermediates conversion efficiency of Co sites, while optimizing H adsorption Gibbs free energy of P sites for HER and OER. The resulting catalyst delivers HER and OER overpotentials of 75 and 373 mV at 10 mA cm−2 in alkaline electrolytes, respectively. The water electrolyzer assembled from CoP/Mo4P3 catalyst can excite 10 mA cm−2 at a low potential of 1.65 V and can be operated for nearly 100 h with excellent stability. This work emphasizes the significance of designing heterostructures with optimized interfaces and hierarchical porosity to advance water splitting technologies.
合理设计双功能异质结构水全面分解催化剂,增强催化剂-电解质界面的电子传递和质量交换,对推进绿色制氢至关重要。本文设计了具有层次(宏-介-微)孔结构的CoP/Mo4P3异质结,在CoP和Mo4P3界面诱导强烈的电子耦合,提高催化稳定性、质量交换效率和活性物质对全水解的利用。在分层多孔的氮掺杂碳多面体中,CoP/Mo4P3通过Mo离子与甘油蚀刻空心ZIF-67之间的阳离子交换生长,然后进行热解和磷化。CoP/Mo4P3异质界面相互作用使电子结构重构,活性位点增加,Co位点的H2O解离能力和中间体转化效率提高,同时优化了HER和OER中P位点的H吸附吉布斯自由能。所得催化剂在碱性电解质中在10 mA cm−2下的HER和OER过电位分别为75和373 mV。由CoP/Mo4P3催化剂组装而成的水电解槽在1.65 V的低电位下可激发10 mA cm−2,并可运行近100 h,稳定性良好。本工作强调了设计具有优化界面和分层孔隙度的异质结构对推进水裂解技术的重要性。
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.