One-Step In Situ Synthesis of a Reduced Graphene Oxide-Based Hybrid Hydrogel for Highly Efficient Water Evaporation and Comprehensive Wastewater Treatment

IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Haining Yang, Wei Li*, Haimin Yang, Ya Xiong, Chengbao Liu, Yongqin Han*, Zhong-Zhen Yu and Xiaofeng Li*, 
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Abstract

Solar-driven wastewater treatment via integrated photothermal evaporation and photocatalysis has emerged as a promising approach for freshwater generation, but it is still a challenge in reconciling the fundamental conflict between charge carrier dynamics, where photothermal conversion inherently promotes electron–hole recombination while photocatalytic reactions demand efficient charge separation for optimal performance. Herein, a reduced graphene oxide/MXene-derived TiO2/polyaniline (GMTP) hydrogel is fabricated, which realizes deep integration of photothermal and photocatalytic performance through multistage carrier pathway engineering and redox potential optimization. The well-designed heterojunction between polyaniline and TiO2 induces the thermalization of low-energy carriers through interfacial recombination to induce solar-to-thermal energy conversion, while spatially segregated high-energy carriers with preserved redox potentials initiate cascade reactions involving •OH and •O2 for contaminant degradation. Density functional theory and electron paramagnetic resonance have validated that the carrier-selective mechanism achieves coordinated enhancement of photothermal conversion efficiency and catalytic activity through quantum-level carrier modulation. As a result, the GMTP evaporator exhibits a high-water evaporation rate of 2.81 kg m–2 h–1 under 1 sun illumination as well as outstanding degradation efficiencies of more than 99% for various organic contaminants without additional oxidants. This multilevel carrier regulation strategy shows great potential in environmental remediation and the applications of relieving the freshwater crisis.

Abstract Image

用于高效水蒸发和综合废水处理的还原氧化石墨烯基杂化水凝胶的一步原位合成。
集成光热蒸发和光催化的太阳能驱动废水处理已成为一种有前途的淡水发电方法,但在协调电荷载流子动力学之间的基本冲突方面仍然存在挑战,其中光热转换本质上促进电子-空穴复合,而光催化反应需要有效的电荷分离以获得最佳性能。本文制备了还原氧化石墨烯/ mxene衍生的TiO2/聚苯胺(GMTP)水凝胶,通过多级载体途径工程和氧化还原电位优化,实现了光热和光催化性能的深度融合。聚苯胺和TiO2之间精心设计的异质结通过界面重组诱导低能载流子的热化,从而诱导太阳能到热能的转换,而空间分离的高能载流子保留氧化还原电位,引发涉及•OH和•O2-的级联反应,从而降解污染物。密度泛函理论和电子顺磁共振验证了载流子选择机制通过量子级载流子调制实现了光热转换效率和催化活性的协同增强。因此,GMTP蒸发器在1个太阳光照下具有2.81 kg m-2 h-1的高蒸发速率,并且在不添加氧化剂的情况下,对各种有机污染物的降解效率超过99%。这种多层次载体调控策略在环境修复和缓解淡水危机方面具有很大的应用潜力。
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来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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