Huang Xin, Du Rui, Zhang Yuanyuan, Ren Jingyu, Yang Qisheng, Wang Kangning, Ni Yang, Yao Yuqi, Ali Soomro Razium, Guo Li, Yang Chunming, Wang Danjun, Xu Bin, Fu Feng
Yan'an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank Coal, College of Chemistry & Chemical Engineering, Yan'an University, Yan'an 716000, PR China.
Yan'an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank Coal, College of Chemistry & Chemical Engineering, Yan'an University, Yan'an 716000, PR China.
J Colloid Interface Sci. 2024 Jun 15;664:33-44. doi: 10.1016/j.jcis.2024.03.018. Epub 2024 Mar 4.
Photocatalytic nitrogen fixation presents an eco-friendly approach to converting atmospheric nitrogen into ammonia (NH), but the process faces challenges due to rapid interface charge recombination. Here, we report an innovative charge transfer and oriented accumulation strategy using an In-O-Mo bond-modulated S-scheme heterostructure composed of InO/BiMoO (In/BMO) synthesized using a simple electrostatic assembly. The unique interfacial arrangement with optimal photocatalyst configuration (3 % In/BMO) enabled enhanced photogenerated electron separation and transfer, leading to a remarkable nitrogen fixation rate of approximately 150.9 μmol·g·h under visible light irradiation. The performance of the photocatalyst was 9-fold and 27-fold higher than that of its pristine components, BiMoO and InO, respectively. The experimental and theoretical evaluation deemed interfacial In-O-Mo bonds crucial for rapid transfer and charge-oriented accumulation. Whereas the generated internal electric field drove the spatial separation and transfer of photo-generated electrons and holes, significantly enhancing the photocatalytic N-to-NH conversion efficiency. The proposed work lays the foundation for designing S-scheme heterostructures with highly efficient interfacial bonds, offering a promising avenue for substantial improvements in photocatalytic nitrogen fixation.
光催化固氮为将大气中的氮转化为氨（NH₃）提供了一种环保方法，但由于界面电荷快速复合，该过程面临挑战。在此，我们报告了一种创新的电荷转移和定向积累策略，该策略使用由In₂O₃/Bi₂MoO₆（In/BMO）组成的In - O - Mo键调制S型异质结构，通过简单的静电组装合成。具有最佳光催化剂构型（3% In/BMO）的独特界面排列能够增强光生电子的分离和转移，在可见光照射下导致约150.9 μmol·g⁻¹·h的显著固氮率。该光催化剂的性能分别比其原始组分Bi₂MoO₆和In₂O₃高9倍和27倍。实验和理论评估认为界面In - O - Mo键对于快速转移和电荷定向积累至关重要。而产生的内电场驱动光生电子和空穴的空间分离和转移，显著提高了光催化N₂到NH₃的转化效率。所提出的工作为设计具有高效界面键的S型异质结构奠定了基础，为大幅提高光催化固氮提供了一条有前景的途径。
