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首页> 外文期刊>Catalysis science & technology >Phase segregation via etching-induced cation migration in CoSx–ZnS nanoarchitectures for solar hydrogen evolution
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Phase segregation via etching-induced cation migration in CoSx–ZnS nanoarchitectures for solar hydrogen evolution

机译：通过蚀刻诱导的阳离子迁移的cosx – ZnS纳米结构中的阳离子迁移的相分离

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摘要

Low charge carrier mobility limits the development of highly efficient semiconductor-based photocatalysis. Heterointerface engineering is a promising approach to spatially separate the photoexcited charge carriers and thus enhance photocatalytic activity. Herein, phase-segregated CoSx–ZnS nanoarchitectures are prepared using a chemically etched hollow ZIF-8 nanoframe (H-ZIF-8) encased by ZIF-67 as a template. Unprecedented dynamic cation migration is observed within the sulfide matrix due to the optimal etching-induced surface energy relieving, offering a clear phase segregation of CoSx and ZnS, which is undiscovered using the unetched ZIF-8@67 dodecahedron as the precursor. Specifically, the heteroepitaxial growth of ZIF-67 on H-ZIF-8 orients the initial cation configuration of Zn2+@Co2+, which is transformed to the sandwich-like Zn2+/Co2+/Zn2+ due to the partially outward diffusion of Zn2+ during the microthermal sulfidation process. The resulting hollow CoSx–ZnS nanoframe with thin shells composed of a ZnS/CoSx/ZnS heterojunction provides three-dimensional accessibility of mass transfer, a large compact heterointerface being beneficial for the promoted charge carrier separation and transfer, and an extended light-absorption region. Consequently, the solar-driven H2 production performance of the CoSx–ZnS hollow nanoframes is greatly enhanced as compared with that derived from unetched ZIFs, and the counterparts ZnS and CoSx. This facile strategy may offer new inspiration for developing more sophisticated nanoarchitectures towards advanced applications.
机译：低电荷载体迁移率限制了高效的半导体光催化的发展。杂截面工程是一种有前途的方法，可以在空间上分离光激发荷载载流子，从而增强光催化活性。本文中，使用ZIF-67包含的化学蚀刻空心ZIF-8纳米装置（H-ZIF-8）作为模板制备了相分解的COSX – ZNS纳米结构。由于最佳蚀刻诱导的表面能缓解，在硫化物基质中观察到了前所未有的动态阳离子迁移，从而提供了COSX和ZnS的清晰相位分离，并以未饲养的ZIF-8@67@67 dodecahedron作为前代的前体进行了清晰的相分离。具体而言，ZIF-67在H-ZIF-8上的异质增生生长呈现Zn2+@CO2+的初始阳离子构型，由于在微疗法硫化过程中Zn2+的部分向外扩散，该Zn2+@CO2+的初始阳离子构型被转化为类似三明治的Zn2+/co2+/Zn2+过程。由Zns/cosx/ZnS杂结组成的薄外壳所得的空心COSX – ZNS纳米架可提供传质的三维可及性，大型紧凑型杂质方面有益于促进的携带载体分离和转移，以及扩展的光吸收区域。因此，与未饲养的ZIF以及对应的Zns和CoSX相比，COSX – ZNS空心纳米框的太阳能驱动的H2生产性能得到了极大的增强。这种便利的策略可能会为开发更复杂的纳米结构提供新的灵感。

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