Synergy between palladium single atoms and small nanoparticles co-anchored on carbon atom self-doped graphitic carbon nitride boosting photocatalytic H2 generation

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-02 DOI:10.1016/j.apcatb.2023.123680

Miao Ren, Jiaqi Meng, Yuxin Yang, Xueyan Zhang, Guang Yang, Lang Qin, Yihang Guo

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Abstract

Supramolecule self-assembly of dicyandiamide and uracil followed by thermal polymerization route is designed to prepare carbon atom self-doped g-C₃N₄ (CCN_x), and then wet reduction is applied to fabricate Pd single atoms (Pd₁) and nanoparticles (Pd_NPs) co-anchored CCN_x heterojunctions (Pd_1+NPs/CCN_x). In Pd_1+NPs/CCN_x structure, interlayer Pd−N₄ coordination is the most favorable for chemically stabilizing Pd₁, while Pd_NPs accumulate on the in-plane of CCN_x. Pd_1+NPs/CCN_x heterojunctions exhibit remarkably enhanced photocatalytic H₂ evolution reaction (HER) activity, and HER rate and AQY value reach up to 24.1 mmol g⁻¹ h⁻¹ and 17.1% (400 nm) over the optimized Pd_1+NPs/CCN_x catalyst. Mechanism studies unveil that synergy of as-built interlayer N−Pd−N electron transfer channels at the atomic-scale and surface Mott–Schottky effect of small Pd nanoparticles notably accelerates migration of photogenerated electrons, which leads to plentiful electrons accumulation around Pd single atoms and small nanoparticles to decrease the energy barrier of H* activation and boost HER photodynamics significantly.

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碳原子自掺杂氮化石墨碳上共锚定的钯单原子和小纳米粒子之间的协同作用促进光催化产生 H2

设计了双氰胺和尿嘧啶的超分子自组装以及热聚合路线制备碳原子自掺杂的 g-C3N4 (CCNx)，然后采用湿还原法制造 Pd 单原子 (Pd1) 和纳米粒子 (PdNPs) 共锚 CCNx 异质结 (Pd1+NPs/CCNx)。在 Pd1+NPs/CCNx 结构中，层间 Pd-N4 配位最有利于 Pd1 的化学稳定，而 PdNPs 则聚集在 CCNx 的面内。在优化的 Pd1+NPs/CCNx 催化剂上，Pd1+NPs/CCNx 异质结表现出显著增强的光催化 H2 演化反应（HER）活性，HER 速率和 AQY 值分别达到 24.1 mmol g-1 h-1 和 17.1% (400 nm)。机理研究表明，原子尺度的层间 N-Pd-N 电子传递通道和小钯纳米颗粒表面的 Mott-Schottky 效应协同作用，显著加速了光生电子的迁移，导致大量电子聚集在钯单原子和小纳米颗粒周围，从而降低了 H* 激活的能垒，显著提高了 HER 光动力学性能。

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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.