石墨烯改性蒙脱石构筑CdS/MoS2光催化材料的多级界面调控及产氢机理研究

The novel photocatalyst is the urgent demand of photocatalytic hydrogen evolution by solar energy. Based on the characteristics of natural clays and the technology of interface adjustment, the water phase dispersity and electron transport efficiency of CdS/MoS2 could be improved, which is an effective way for improving photocatalytic performances and reducing the cost. This project aims to in-situ construct CdS/MoS2 composite photocatalytic materials supported on conductive graphene modified montmorillonite via one-pot hydrothermal method, based on the nanosheet-like morphology and excellent hydrophilicity of montmorillonite. Through the hydrogen bonding between the surface hydroxyl and synergistic coupling effect of doped S atom, multistage interfaces of montmorillonite-graphene-CdS/MoS2 could be adjusted. In this project, we will illuminate the structure evolution rule and interfacial adjustment mechanism in the construct process, and improve the structure stability and photocatalytic performance by optimum process. Combining experimental characterization and computational simulation, we will establish the microstructure model of composite photocatalytic materials. The electron transport pathways of catalytic reaction are studied, and the synergetic enhancement mechanism for hydrogen producing performance is revealed. The relationship between the microstructures and the photocatalytic performances of the composites is found, and the theoretical principles for the controlled preparation and performance optimization of montmorillonite-based photocatalytic materials are established. The accomplishment of the project could offer a novel idea for the hydrogen evolution technology with high performance and low cost, and show important scientific significance and practical value for the high-valued applications of mineral resources as well.

针对太阳能光解水制氢对新型光催化剂的迫切需求，利用粘土矿物的天然特性和界面调控技术，提高CdS/MoS2的水相分散性和电子传输效率，是增强材料光催化性能并降低成本的有效途径。本项目基于蒙脱石的纳米片状形貌和优良亲水性，以高导电性的石墨烯表面改性，采用一步水热法原位负载CdS/MoS2，构筑蒙脱石基光催化材料。通过表面羟基之间氢键和掺杂硫原子协同耦合效应，实现蒙脱石-石墨烯-CdS/MoS2之间的多级界面调控，阐明材料构筑过程中的结构演变规律和界面调控机制，优化工艺提高材料结构稳定性和光催化性能。结合实验表征和计算模拟，构建复合材料的微观结构模型，研究催化反应的电子传输途径，揭示产氢性能的协同增强机理，建立材料微结构与光催化性能的构效关系，确立蒙脱石基光催化材料可控制备和性能优化的理论原则。本项目的完成可为高性能、低成本产氢技术提供新思路，对矿物资源的高值化利用具有重要的科学意义和实用价值。

太阳能光催化分解水制氢是清洁能源领域的重大前沿方向，其关键技术是设计开发高性能、低成本的新型光催化材料。本项目以石墨烯改性蒙脱石为载体材料，负载CdS/MoS2，构筑蒙脱石基复合光催化材料，研究复合材料的多级界面调控机制和产氢机理。具体研究内容包括：蒙脱石复合CdS/MoS2光催化材料的构筑与性能优化，蒙脱石基复合催化材料的多级界面调控与机制分析，石墨烯改性蒙脱石构筑CdS/MoS2光催化材料的产氢性能与机理研究，粘土矿物复合过渡金属硫化物催化材料体系的探索与应用。研究发现：一步水热法制备的CdS纳米颗粒/MoS2纳米片异质结构均匀负载在蒙脱石上，调节CdS/MoS2比例可优化复合材料的光催化性能；石墨烯或碳材料改性蒙脱石可获得亲水导电的催化载体，复合催化材料的多级界面结构有利于提高材料结构稳定性和催化性能；石墨烯改性蒙脱石构筑CdS/MoS2光催化材料性能优异，具有广阔的应用前景，其中蒙脱石提高复合材料水相分散性，石墨烯提高电子传输效率，CdS作为光催化剂，MoS2提供产氢催化活性位点，复合材料各组元协同增强光催化产氢性能；粘土矿物负载过渡金属硫化物催化剂表现出明显的形貌效应，二维粘土纳米片负载MoS2具有更好的形貌优势，复合催化材料体系在电催化产氢和环境催化领域也表现出巨大潜力。本项目的研究结果扩展了粘土矿物复合材料的应用领域，为高性能、低成本光催化材料设计提供新思路，对矿物资源的高值化利用具有重要的理论和实用价值。