Tiwei He, Hongchao Tang, Jie Wu, Jiaxuan Wang, Mengling Zhang, Cheng Lu, Hui Huang, Jun Zhong, Tao Cheng, Yang Liu, Zhenhui Kang
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引用次数: 0
摘要
碳基无金属催化剂因其低成本和环保性而成为光催化和电催化领域前景广阔的绿色催化剂。由于这些催化剂结晶度低、结构复杂,利用这些催化剂的一个关键挑战是确定其活性位点。在这里,我们展示了双键共轭碳基作为无金属活性位点的关键结构,通过级联水氧化-O2还原过程将 O2 高效光还原为 H2O2。我们以乙二胺四乙酸为前驱体,合成了多种碳基光催化剂,并分析了它们的结构演变。在 260 °C 至 400 °C 的聚合条件下,催化剂表面形成了类似 N-乙基-2-哌嗪酮的结构,从而在可见光下产生了较高的光催化 H2O2 光生成率(2884.7 μmol g-1h-1)。一系列对照实验和理论计算进一步证实,双键共轭羰基结构是无金属光催化剂活性位点的关键和普遍特征。
A metal-free cascaded process for efficient H2O2 photoproduction using conjugated carbonyl sites.
Carbon-based metal-free catalysts are promising green catalysts for photocatalysis and electrocatalysis due to their low cost and environmental friendliness. A key challenge in utilizing these catalysts is identifying their active sites, given their poor crystallinity and complex structures. Here we demonstrate the key structure of the double-bonded conjugated carbon group as a metal-free active site, enabling efficient O2 photoreduction to H2O2 through a cascaded water oxidation - O2 reduction process. Using ethylenediaminetetraacetic acid as a precursor, we synthesized various carbon-based photocatalysts and analyzed their structural evolution. Under the polymerization conditions of 260 °C to 400 °C, an N-ethyl-2-piperazinone-like structure was formed on the surface of the catalyst, resulting in high photocatalytic H2O2 photoproduction (2884.7 μmol g-1h-1) under visible light. A series of control experiments and theoretical calculations further confirm that the double-bond conjugated carbonyl structure is the key and universal feature of the active site of metal-free photocatalysts.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.