Nano Energy ( IF 16.8 ) Pub Date : 2020-09-19 , DOI: 10.1016/j.nanoen.2020.105401 Mengyang Xia , Xiaoqing Yan , He Li , Nathan Wells , Guidong Yang
La2Ti2O7, a layered perovskite material, has attracted much attention in photocatalytic hydrogen production due to its high stability and non-toxic. Combing La2Ti2O7 with narrow band gap semiconductors to construct 2D/2D heterojunction is a facile strategy to improve photocatalytic activity. In this work, we first report a novel 2D/2D N–La2Ti2O7/ZnIn2S4 heterojunction via in-situ growth of abundant well-dispersed ZnIn2S4 nanosheets on the N–La2Ti2O7 nanosheets surface. Experimental results show the optimized 2D/2D N–La2Ti2O7/ZnIn2S4 sample exhibits the best light-driven H2 evolution activity, which is nearly 5.2 and 1.7 times higher than that of pristine ZnIn2S4 and 2D/2D La2Ti2O7/ZnIn2S4 samples, respectively. This is due to the unique 2D/2D heterojunction produces high-speed charge transfer channels, thus significantly enhancing photo-carriers separation and migration efficiency. Meanwhile, DFT calculations confirm nitrogen doping forms impurity energy states at the top of valence band, thus narrowing the band gap of La2Ti2O7, considerably inhibiting electron-hole pair recombination. Further the microstructures and charge separation properties are analyzed by SEM, PL, and DFT calculations to reveal the structure-activity relationship of hetero-structure and the synergistic mechanism of each functional component. This report will hopefully provide a practical strategy for designing heterojunction composite for high light-driven hydrogen evolution rate.
中文翻译:
通过能带结构/形态调控协同效应,精心设计的2D / 2D N掺杂La 2 Ti 2 O 7 / ZnIn 2 S 4异质结中有效的电荷分离
层状钙钛矿材料La 2 Ti 2 O 7,由于其高稳定性和无毒性而在光催化制氢中引起了广泛关注。将La 2 Ti 2 O 7与窄带隙半导体结合在一起以构建2D / 2D异质结是提高光催化活性的简便策略。在这项工作中,我们首先报道了一种新的2D / 2D的N-的La 2的Ti 2 ö 7 /日宁2小号4经由丰富良好分散的日宁的原位生长异质结2小号4纳米片在N的La 2的Ti 2 ö7纳米片表面。实验结果表明,优化的2D / 2D N–La 2 Ti 2 O 7 / ZnIn 2 S 4样品具有最佳的光驱动H 2析出活性,比原始ZnIn 2 S 4和ZnIn 2 S 4分别高近5.2和1.7倍。2D / 2D La 2 Ti 2 O 7 / ZnIn 2 S 4样本。这是由于独特的2D / 2D异质结产生了高速电荷转移通道,从而显着提高了光电载流子的分离和迁移效率。同时,DFT计算证实了氮掺杂在价带的顶部形成杂质能态,从而缩小了La 2 Ti 2 O 7的带隙。,大大抑制了电子-空穴对的重组。通过SEM,PL和DFT计算进一步分析了微结构和电荷分离特性,揭示了异质结构的构效关系和各功能组分的协同机理。该报告有望为设计高光驱氢释放速率的异质结复合材料提供实用的策略。