Wang Shikai, Zhang Dong, Pu Xipeng, Zhang Lizhi, Zhang Dafeng, Jiang Jizhou
School of Materials Science and Engineering, Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, and School of Physics Science and Information Technology, Shandong Key Laboratory of Optical Communication Science and Technology, Liaocheng University, Liaocheng, Shandong, 252000, P. R. China.
School of Environmental Ecology and Biological Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan, 430205, P. R. China.
Small. 2024 Jul;20(30):e2311504. doi: 10.1002/smll.202311504. Epub 2024 Feb 27.
Herein, guided by the results of density functional theory prediction, the study rationally designs a hollow core-shell FeNiS@ZnInS (FNS@ZIS) Step-scheme (S-scheme) heterojunction for photocatalytic H evolution with photothermal-assisted. The hollow FNS spheres offered substrate for coating the ZIS nanosheets, which can inhibit ZIS nanosheets from agglomerating into pellet, enrich the active site, increase specific surfaces, and raise the light absorption. Notably, due to its excellent photothermal properties, FNS core generated heat unceasingly inside under visible-light irradiation and effectively prevent the heat loss of the reaction system, which increased the local temperature of photocatalysts and thus accelerated the charge migration. In addition, the S-scheme heterojunction construction via in situ growth has a tight interface, which can facilitate the separation and transfer of carriers and achieve high redox potential. Owning to the distinctive construction, the hollow core-shell FNS@ZIS S-scheme heterojunction show extraordinary stability and photocatalytic H evolution rate with 7.7 mmol h g, which is ≈15.2-fold than pristine ZIS. Based on the double evidence of theoretical predictions and experimental confirmations, the photothermal effect and electron transfer mechanism of this innovative material are investigated in depth by the following infrared thermography technology and deep DFT calculations.
在此，在密度泛函理论预测结果的指导下，本研究合理设计了一种空心核壳结构的FeNiS@ZnInS（FNS@ZIS）型异质结，用于光热辅助光催化析氢。空心的FNS球体为ZIS纳米片的包覆提供了基底，能够抑制ZIS纳米片团聚成颗粒，富集活性位点，增加比表面积，并提高光吸收。值得注意的是，由于其优异的光热性能，FNS核在可见光照射下不断在内部产生热量，并有效防止反应体系的热量损失，这提高了光催化剂的局部温度，从而加速了电荷迁移。此外，通过原位生长构建的S型异质结具有紧密的界面，能够促进载流子的分离和转移，并实现高氧化还原电位。由于其独特的结构，空心核壳FNS@ZIS S型异质结表现出非凡的稳定性和光催化析氢速率，达到7.7 mmol h g，约为原始ZIS的15.2倍。基于理论预测和实验验证的双重证据，通过以下红外热成像技术和深度密度泛函理论计算，对这种创新材料的光热效应和电子转移机制进行了深入研究。
