Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)

IF 2.7 4区化学 Q3 CHEMISTRY, PHYSICAL Electrocatalysis Pub Date : 2023-11-11 DOI:10.1007/s12678-023-00852-9

Sirlon F. Blaskievicz, Ivo F. Teixeira, Lucia H. Mascaro, Mariolino Carta, Neil B. McKeown, Yuanzhu Zhao, Frank Marken

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Abstract

Polymeric carbon nitrides (C₃N₄) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell.

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镍改性聚(庚嗪酰亚胺)的氢介导光电催化作用

聚合碳氮化物（C3N4）是一种具有光化学活性的有机半导体，可制成多种结构类型。在此，我们将含有镍单原子（Ni-PHI）的聚庚嗪亚胺用于光化学制氢，并与不掺镍的半导体进行比较。在铂盘电极（检测氢气）上形成薄膜沉积，然后涂上一层具有固有微孔的分子刚性聚合物 PIM-1，以便 (i) 在不妨碍光催化的情况下机械地稳定光催化剂薄膜，(ii) 协助界面氢捕获/氧抑制过程。在存在甲醇或乙醇等空穴淬灭剂的情况下，可观察到与氢产生/氧化有关的阳极光电流。与在玻璃碳上进行的实验相比较，证实了界面氢作为介质的形成。评估了空穴淬灭剂浓度的影响。在单室光燃料电池中采用了 Pt/Ni-PHI/PIM-1 系统。

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来源期刊

Electrocatalysis CHEMISTRY, PHYSICAL-ELECTROCHEMISTRY

CiteScore

4.80

自引率

6.50%

发文量

审稿时长

>12 weeks

期刊介绍： Electrocatalysis is cross-disciplinary in nature, and attracts the interest of chemists, physicists, biochemists, surface and materials scientists, and engineers. Electrocatalysis provides the unique international forum solely dedicated to the exchange of novel ideas in electrocatalysis for academic, government, and industrial researchers. Quick publication of new results, concepts, and inventions made involving Electrocatalysis stimulates scientific discoveries and breakthroughs, promotes the scientific and engineering concepts that are critical to the development of novel electrochemical technologies. Electrocatalysis publishes original submissions in the form of letters, research papers, review articles, book reviews, and educational papers. Letters are preliminary reports that communicate new and important findings. Regular research papers are complete reports of new results, and their analysis and discussion. Review articles critically and constructively examine development in areas of electrocatalysis that are of broad interest and importance. Educational papers discuss important concepts whose understanding is vital to advances in theoretical and experimental aspects of electrochemical reactions.