Bioinspired electron carrier mediated transmembrane photocatalytic hydrogen evolution in silica colloidosomes†

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Chengkun Bai, Bingdi Wang, Zhengshun Jiang, Chunying Lv, Zhenning Liu, Shiyu Wang, Song Liang and Hongying Zang
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Abstract

Inspired by the ordered processes of chloroplasts in photosynthesis involving coordinative linkages and efficient compartmentalization, a bioinspired compartmentalized photocatalytic system (BCPS) with an inorganic compartment is designed for photocatalytic hydrogen evolution with light driven electron carrier mediated cross-membrane energy transport. A typical BCPS comprises silica colloidosomes containing co-catalysts as microreactors, where positively charged N-methyl-4-cyanopyridinium (MCP+) serves as the electron carrier. The MCP+ molecules harvest energy from photoexcited g-C3N4, and transit to electrically neutral species MCP0, which can pass the colloidosome. Driven by light, the MCP0 diffuse across the membrane and transport electrons to H+ for hydrogen evolution, in which Pt particles are employed as co-catalysts. Analogous to natural photosynthesis, hydrogen evolution occurs within compartments, separating light and dark reactions, protecting the dark reaction from interference during light harvesting and minimizing potential side effects. The system enables sustained evolution of hydrogen with a higher yield than that with the control catalysis in a bulk catalyst suspension. The dramatic influence of SDS on the hydrogen evolution was revealed, and a possible mechanism of electron carrier amount buffering was proposed.

Abstract Image

硅胶胶体中生物启发电子载体介导的跨膜光催化氢气进化
受叶绿体在光合作用中涉及协调联系和高效区隔的有序过程的启发,设计了一种带有无机区隔的生物启发光催化系统(BCPS),用于光催化氢气进化,光驱动电子载体介导跨膜能量传输。典型的 BCPS 由含有辅助催化剂的二氧化硅胶体作为微反应器组成,其中带正电荷的 N-甲基-4-氰基吡啶鎓(MCP+)作为电子载体。MCP+ 分子从被光激发的 g-C3N4 中获取能量,并转化为电中性物质 MCP0,后者可以通过胶体。在光的驱动下,MCP0 跨膜扩散,利用铂辅助催化剂将电子传递给 H+,从而产生氢气。与自然光合作用类似,氢气进化发生在隔间内,将光反应和暗反应分开,保护暗反应在光收集过程中不受干扰,并将潜在的副作用降至最低。该系统可实现持续的氢气进化,其产率高于在散装催化剂悬浮液中进行的对照催化。研究揭示了 SDS 对氢气进化的巨大影响,并提出了电子载体量缓冲的可能机制。
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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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