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.

Graphical Abstract

Abstract Image

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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

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