| 郑会勤,樊耀亭.“开放型蝶形”[2Fe2S]化合物光催化产氢性能与机理探究[J].分子催化,2023,37(4):331-341 |
| “开放型蝶形”[2Fe2S]化合物光催化产氢性能与机理探究 |
| Study of Photocatalytic Hydrogen Production Performance and Mechanism of ‘Open Butterfly’ [2Fe2S] Compounds |
| 投稿时间：2023-02-21 修订日期：2023-03-23 |
| DOI：10.16084/j.issn1001-3555.2023.04.002 |
| 中文关键词: [2Fe2S]化合物 光催化产氢 电化学 荧光淬灭 机理 |
| 英文关键词:[2Fe2S] compounds photocatalytic hydrogen production electrochemistry fluorescence quenching mechanism |
| 基金项目:国家自然科学基金项目(No.21171147);河南省青年骨干教师项目(No.2020GGJS266);河南省高等学校重点科研项目(No.21B150001) |
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| 中文摘要: |
| 合成并表征了两个新的具有 “开放型蝶形” 结构的[2Fe2S]化合物A和B; 并以A和B为催化剂、 藻红B钠盐 (EBS2-) 为光敏剂、 三乙胺 (TEA) 为电子给体和质子源, 构建了一个均相光催化产氢体系. 结果表明: 体系在pH为12, 体积比为1∶1的CH3CN/H2O溶液中，产氢活性最高，经4 h可见光照射，最大产氢量分别为156.1 μmol (37.9 TON vs. A) 和18.4 μmol (TON 4.6 vs. B); 催化剂中含有质子捕获位点, 有利于形成产氢活性中间体H2-Fe2S2(η2-H2-FeIIFeI) 物种, 从而提高催化剂的产氢活性. 在当前的体系中, 还原态的 FeIFe0 物种通过1* EBS2-转移到FeIFeI中心上, 然后再经历一个EECC (化合物A) 或ECEC (化合物B), 形成产氢活性中间体H2-Fe2S2(η2-H2-FeIIFeI)物种, 最终产生H2分子, 并使FeIFeI 物种再生. |
| 英文摘要: |
| Two new compounds A and B with ‘open butterfly’ structure [2Fe2S] compounds were synthesized and characterized. Then, a homogeneous photocatalytic hydrogen production system was constructed, among which complex A or B, EBS2- and TEA was used as catalysts, photosensitizer, and electron donor & proton source, respectively. The results show that the hydrogen production activity is the highest in the CH3CN∶H2O solution with a pH of 12 and a volume ratio of 1∶1. The maximum hydrogen production is 156.1 μmol (37.9 TON, turn over number) vs. A) and 18.4 μmol (TON 4.6 vs. B) in 4 hours of visible light irradiation; the catalyst contains proton trapping sites, which are conducive to the formation of hydrogen-producing active intermediate H2-Fe2S2 (η2-H2-FeIIFeI) species, thereby improving the hydrogen-producing activity. In the current system, the reduced FeIFe0 species is transferred from 1*EBS2- to the FeIFeI center, and then undergoes an EECC (Compound A , electron-transfer process (E) , Chemical reaction process(C)) or ECEC (Compound B) to form the hydrogen-producing the above active intermediate species, eventually producing H2 molecules and regenerating the FeIFeI species. |
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