A dual-functional supramolecular assembly for enhanced photocatalytic hydrogen evolution

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2022-09-05 DOI:10.1016/j.apcatb.2022.121386

Lin Qin, Ruijie Wang, Xing Xin, Mo Zhang, Tianfu Liu, Hongjin Lv, Guo-Yu Yang

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Abstract

The construction of multifunctional supramolecular assembly is a central research interest in solar-driven water splitting to hydrogen. We here report the successful preparation of a dual-functional supramolecular assembly via facile electrostatic integration of a positively-charged Ir-based chromophore and a negatively-charged nickel-substituted polyoxometalate catalyst. The resulting dual-functional supramolecule can form ordered vesicle-like assemblies and work efficiently as both light-absorber and catalyst for hydrogen production under visible light irradiation. Under minimally optimized conditions, a catalytic hydrogen production turnover number of over 4000 was achieved after 96-hour irradiation, which is 17 times to that of discrete components under otherwise identical conditions. Destruction of such ordered vesicle-like assemblies will lead to a remarkable decrease of photocatalytic hydrogen production activity. Mechanistic studies further revealed the presence of both oxidative and reductive quenching processes during photocatalysis and also confirmed that the formation of ordered supramolecule is beneficial for effective electron transfer between chromophore and catalyst.

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用于增强光催化析氢的双功能超分子组件

多功能超分子组装的构建是太阳能驱动水分解成氢的核心研究兴趣。我们在这里报道了通过一个带正电的ir基发色团和一个带负电的镍取代的多金属酸盐催化剂的静电集成，成功制备了一个双功能超分子组装体。所得到的双功能超分子可以形成有序的囊泡状组装体，并在可见光照射下高效地作为光吸收剂和催化剂产氢。在最小优化条件下，经过96小时的辐照，催化制氢周转率达到4000以上，是其他条件下离散组分的17倍。这种有序的囊泡样组装体的破坏将导致光催化产氢活性的显著降低。机理研究进一步揭示了光催化过程中存在氧化和还原性猝灭过程，也证实了有序超分子的形成有利于发色团和催化剂之间有效的电子转移。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.