一个由布里斯托大学Ian Manners课题组领导的国际合作小组，通过自组装纳米纤维实现了可见光驱动的高效产氢。 2020年11月20日出版的《自然—化学》发表了这项成果。
创造能模拟自然光合作用的高效人工光合系统是当前的一个重要科学挑战。在本文中，研究人员描述了一种高性能、可重复使用的光催化核-壳结构纳米纤维系统，该系统通过将一种钴催化剂和光敏剂紧密集成在一起，实现了水的可见光催化产氢。纳米纤维的组成、微观结构和尺寸——以及由此产生的催化活性——都是通过活性结晶驱动的自组装来控制的。在这个由种子引发的生长策略中，具有可结晶的成核嵌段与功能性冠状片段的嵌段共聚物在一起组装成低分散度的一维结构。
在最佳条件下，该纳米纤维可促进水光解产氢，其太阳能转化为氢气的总量子效率约为4.0%。在1.34微克材料的催化下，该反应转换数在五小时间大于7000，相当于大于1400的每小时转换数和大于0.327 μmol h−1的氢气产率（即>244300 μmol·h-1/每克催化材料）。
附：英文原文
Title: Tailored self-assembled photocatalytic nanofibres for visible-light-driven hydrogen production
Author: Jia Tian, Yifan Zhang, Lili Du, Yunxiang He, Xu-Hui Jin, Samuel Pearce, Jean-Charles Eloi, Robert L. Harniman, Dominic Alibhai, Ruquan Ye, David Lee Phillips, Ian Manners
Issue&Volume: 2020-11-20
Abstract: The creation of efficient artificial systems that mimic natural photosynthesis represents a key current challenge. Here, we describe a high-performance recyclable photocatalytic core–shell nanofibre system that integrates a cobalt catalyst and a photosensitizer in close proximity for hydrogen production from water using visible light. The composition, microstructure and dimensions—and thereby the catalytic activity—of the nanofibres were controlled through living crystallization-driven self-assembly. In this seeded growth strategy, block copolymers with crystallizable core-forming blocks and functional coronal segments were coassembled into low-dispersity, one-dimensional architectures. Under optimized conditions, the nanofibres promote the photocatalytic production of hydrogen from water with an overall quantum yield for solar energy conversion to hydrogen gas of ~4.0% (with a turnover number of >7,000 over 5 h, a frequency of >1,400 h−1 and a H2 production rate of >0.327 μmol h−1 with 1.34 μg of catalytic polymer (that is, >244,300 μmol h−1 g−1 of catalytic polymer)).
DOI: 10.1038/s41557-020-00580-3
Source: https://www.nature.com/articles/s41557-020-00580-3
期刊信息
Nature Chemistry：《自然—化学》，创刊于2009年。隶属于施普林格·自然出版集团，最新IF：21.687
