Zhang Meng, Chen Xujian, Jiang Xinyan, Wang Jin, Xu Liyun, Qiu Junhao, Lu Wenrong, Chen Deli, Li Zhengquan
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Normal University, Jinhua, Zhejiang 321004, P. R. China.
ACS Appl Mater Interfaces. 2021 Mar 31;13(12):14198-14206. doi: 10.1021/acsami.0c22869. Epub 2021 Mar 21.
Developing suitable catalysts capable of receiving injected electrons and possessing active sites for hydrogen evolution reaction (HER) is the key to building an efficient dye-sensitized system for hydrogen production. FeS is generally regarded as an inferior HER catalyst among the metal sulfide family, mainly due to its weak surface adsorption toward H atoms. In this work, we demonstrate a facile metal-organic framework-derived method to synthesize uniform FeS nanorods and active them for HER by Ni doping. Our experimental results and theoretical calculations reveal that Ni doping can greatly modify the electronic structure of FeS nanorods, improving their electron conductivity and optimizing their surface adsorption energy toward H atoms. Sensitized by a commercial organic dye (eosin-Y), 1%Ni-doped FeS nanorods display a high H production rate of 3240 μmol g h with an apparent quantum yield of 12% under 500 nm wavelength, which is significantly higher than that of pristine FeS and even higher than that of 1% Pt-deposited FeS. The working mechanism of this dye-sensitized system is explored, and the effect of Ni-doping concentration has been studied. This work presents a facile strategy to synthesize metal-doped sulfide nanocatalysts with greatly enhanced activity toward photocatalytic H production.
开发能够接收注入电子并具有析氢反应(HER)活性位点的合适催化剂是构建高效染料敏化制氢系统的关键。在金属硫化物家族中,FeS通常被认为是一种较差的HER催化剂,主要是因为其对H原子的表面吸附较弱。在这项工作中,我们展示了一种简便的金属有机框架衍生方法来合成均匀的FeS纳米棒,并通过Ni掺杂使其具有HER活性。我们的实验结果和理论计算表明,Ni掺杂可以极大地改变FeS纳米棒的电子结构,提高其电子导电性并优化其对H原子的表面吸附能。由商业有机染料(曙红-Y)敏化,1%Ni掺杂的FeS纳米棒在500 nm波长下显示出3240 μmol g h的高产氢率,表观量子产率为12%,这明显高于原始FeS,甚至高于1%Pt沉积的FeS。探索了该染料敏化系统的工作机制,并研究了Ni掺杂浓度的影响。这项工作提出了一种简便的策略来合成对光催化产氢具有大大增强活性的金属掺杂硫化物纳米催化剂。