二维半导体可见光光催化剂的设计与性能调控是当前新能源和新材料研究领域的前沿课题之一，而如何综合突破多种主要反应限制因素的制约则是有效提升材料光催化水分解性能亟待解决的重要科学问题。有鉴于此，本项目选取具有高稳定性的原子级厚超薄LNS-TiO2纳米片作为研究对象，首次提出利用二元错层补偿共掺杂的方法实现复合双层结构纳米片的高活性可见光光催化水分解能力。结合高通量第一性原理计算和实验验证反馈，探索共掺杂元素组合的协同效应综合改善材料光学吸收、氧化还原能力、光生载流子分离和表面反应位点活性等基本因素的潜在规律。同时，借助电子轨道相互作用为桥梁，揭示相关影响规律的微观机制起源，建立适用于二维材料光催化性能调控的前瞻性物理模型。本项目拟取得的系统性成果对于高效可见光光催化剂的设计和潜在应用具有重要的科学意义。

Designing and tuning properties of 2D semiconductor photocatalysis is one of the hot topics in the fields of new energy and materials. And how to simultaneously overcome the basic restrictions of water splitting is the important scientific issue for effectively enhancing the photocatalytic properties of materials. On this account, this project focuses on the atomic-thick LNS-TiO2 nanotheets with high stability. The strategy of bilayer LNS-TiO2 nanosheet with compensated codoping in separated layers is firstly proposed to realize the visible-light photocatalytic water splitting. Combining the high-through first principle calculations and experimental feedback, the potential relationship between the synergistic effect of codoping elements and factors for photocatalytic water splitting reaction, such as optical adsorption, oxidation and reduction potentials, photon-generated carriers separation, and activity of surface reaction center, will be systematically explored. And, based on the electronic orbital interaction, the micromechanics of the above relationship will be analyzed. More importantly, the forward physical model will be built for photocatalytic properties modulation of 2D materials. Therefore, the achievements from this project will exhibit high scientific significance for the design and application of new visible-light photocatalysis with high efficiency.