P, N-codoped carbon nanofibers confined ultra-small bimetallic NiCoP for highly efficient overall water splitting
P, N-codoped carbon nanofibers confined ultra-small bimetallic NiCoP for highly efficient overall water splitting
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P、N共掺杂碳纳米纤维约束超小型双金属NiCoP，实现高效整体水分解
DOI：
10.1016/j.apsusc.2021.151247
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发表时间：
2021-12
影响因子：
6.7
通讯作者：
Jianhua He
中科院分区：
文献类型：
--
作者：
Xueping Sun;Peng Wei;Jinxu Zhang;Songqi Gu;Ruoou Yang;Chun Fang;Qing Li;Jiantao Han;Zheng Jiang;Jianhua He
由于单磷化物具有独特的类金属性质和活性中心的局部电子/几何结构，单磷化物已成为水裂解反应的理想催化剂，但由于合成方法的毒性、腐蚀性和高温性，导致单磷化物的粒径增大，催化活性降低.本文以植酸为辅助剂，采用静电纺丝法成功制备了P，N共掺杂纳米碳纤维原位包埋超细NiCoP催化剂（NiCoP@PNCNF）。通过独特的宏观结构设计和微电子/几何修饰，所制备的NiCoP@PNCNF催化剂表现出优异的HER（η10= 98 mV）和OER（η10= 260 mV）催化性能，表现出较低的过电位和在碱性溶液中的稳定性。同时，XAFS分析进一步表明，显着的催化性能不仅归功于杂原子掺杂碳纤维的引入，提高了其耐腐蚀性、抗团聚能力和导电性，而且还得益于Ni/Co之间的强协同作用，局部电子/几何结构的变化和P原子的作用。在实际应用中，还研究了基于NiCoP@PNCNF电极的水裂解性能，并在长期稳定性测试中显示出较低的裂解电位（EJ= 10，1.645 V）。这些富有洞察力的发现无疑为设计和制造具有成本效益和鲁棒性的双功能过渡金属磷化物电催化剂提供了启示。
Integrating the unique metalloid behaviour of monometallic phosphides and modified local electronic/geometric structures of active sites, bimetallic phosphides have emerged as promising candidates for water splitting reaction, but they are still synthesized by toxic, corrosive, and high-temperature methods, which inevitably resulted in an increase of particle size and the decrease of catalytic activity area. Herein, the ultra-fine bimetallic NiCoP catalysts in-situ embedded in P, N-codoped carbon nanofibers (NiCoP@PNCNF) were successfully fabricated via a facile electrospinning method with the help of phytic acid. Profiting from the unique macro-structural design and micro-electronic/geometric modification, as-prepared NiCoP@PNCNF catalysts exhibited excellent catalytic performance both for HER (η10= 98 mV) and OER (η10= 260 mV) in terms of the low overpotential and robust stabilities in alkaline solution. Meanwhile, XAFS analysis further demonstrated that the remarkable catalytic performance not only attributed to the introduction of heteroatom-doped carbon fibers as their improvements in the corrosion resistance, anti-agglomeration abilities, and conductivity, but also benefited from the local electronic/geometric structure alternations as the strong synergic effects between Ni/Co and P atoms. For practical application, the water splitting performance based on NiCoP@PNCNF electrodes was also investigated and exhibited a lower splitting potential (EJ=10,1.645 V) over long-term stability tests. These insightful findings undoubtedly shed light on the design and fabrication of cost-effective and robust bifunctional transition-metal phosphides electrocatalysts.
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