剑桥大学刘永鹏/Erwin Reisner团队JACS:Z型半人工光合作用系统
学术
2024-10-17 20:03
上海
在光催化领域中,将半导体与生物催化剂(例如酶,细菌等)相结合的半人工光合作用系统是一种极具前景的太阳能燃料生产技术。然而,目前酶光催化系统普遍离不开电子/空穴牺牲剂的使用。有鉴于此,剑桥大学刘永鹏、Erwin Reisner报道了一种新型的Z型半人工光合作用系统能在仅使用水作为电子给体的情况下进行全解水和二氧化碳还原。1.构建了以酶作为助催化剂的Z型光催化系统。此Z型光催化系统由氧化钌修饰的钼掺杂钒酸铋、硫酸·三-2,2′-联吡啶合钴(II)、镧铑共掺杂的钛酸锶、氢化酶、甲酸脱氢酶所组成。 2.研究人员通过Z型光催化半反应实验发现产物的饱和现象是由二价钴电子媒介的氧化耗尽所引起。3. 在模拟太阳光照条件下Z型光催化全反应实验表明此系统能稳定生产氢气或甲酸10小时并未出现半反应中产物饱和的情况,证明钴基电子媒介可以被重复的氧化和还原重新生成。氢气和甲酸的转化频率分别达到5055每小时和1274每小时,均为Z型光催化中的最高值。4.一系列的电化学测试结果表明钴基电子媒介的工作稳定性在20小时以上。 5. 石英晶体微天平测试揭示了氢化酶与甲酸脱氢酶在镧铑共掺杂的钛酸锶上的吸附/脱附过程。6. 光电化学阻抗谱、瞬时光电流谱、强度调制光电压谱揭示了光生载流子的传输机制。 刘永鹏,2015年在华中科技大学获学士学位,2016年在格拉斯哥大学获硕士一等荣誉学位,2021年8月毕业于在瑞士洛桑联邦理工大学获化学与化学工程博士学位,2021年9月至12月在日内瓦大学从事访问学者工作。获瑞士国家基金委(SNSF)、艾萨克•牛顿信托基金会(INT)、利华休姆信托基金会(Leverhulme Trust)资助,2022年1月至今在剑桥大学化学系Prof. Erwin Reisner课题组开展博士后研究,方向为bio-hybrids。相关研究成果以34篇学术论文的形式发表于Nat. Catal.,JACS(4),JACS Au,Angew. Chem.(2),Chem. Sci.,EES,Adv. Mater.,AFM,ACS Energy Letter.,ACS Nano, JMCA(4)等国际期刊,近5年来发表第一/共一作者13篇,通讯作者3篇,h因子为18。作为独立审稿人,为Adv. Mater.,Joule,ACS Energy Letter.,JMCA,iScience,ChemSusChem,SolarRRL等杂志审稿30余次。近3年来主持项目经费总计近300万元。1. 利华休姆信托基金会Early Career Fellowship(2024-2027,88万)2. 艾萨克•牛顿信托基金会Matching Fund(2024-2027,72万) 3. 艾萨克•牛顿信托基金会Early Career Fellowship(2024,25万)4. 瑞士国家基金委Postdoc.Mobility(2022-2023,97万)1. 瑞士国家基金委Ambizione Energy(2017-2020,625万)Erwin Reisner is the Professor of Energy and Sustainability in the Department of Chemistry at the University of Cambridge and a Fellow of St. John’s College. He is an expert in renewable energy and sustainable chemistry, in particular the sunlight-powered production of sustainable fuels and platform chemicals. His cross-disciplinary research into solar chemical synthesis technologies focuses on the capture and utilisation of the greenhouse gas carbon dioxide as well as the valorisation of plastics and biomass waste to produce green fuels and chemicals for a circular economy.Erwin’s research on solar chemical synthesis has been supported and recognised by several grants, such as an EPSRC Career Acceleration Fellowship (2009-2015), the Christian Doppler Laboratory for Sustainable SynGas Chemistry (2012-2019), a European Research Council (ERC) Consolidator Grant (2016-2023) and an ERC/UKRI Advanced Grant (2023-2028), as well as awards, such as the Corday-Morgan Prize by the Royal Society of Chemistry (2018), the Galvani Prize of the Bioelectrochemical Society (2022) and the Hughes Medal by the Royal Society (2023). He is the academic lead (PI) of the Cambridge Circular Plastics Centre (CirPlas; since 2019), co-director of the Centre for Doctoral Training in Integrated Functional Nano (nanoCDT) in Cambridge, and has previously acted as the academic lead of the UK Solar Fuels Network, which coordinates the national activities in artificial photosynthesis (2017-2021).
Yongpeng Liu, et al., Solar Fuel Synthesis Using a Semiartificial Colloidal Z‑Scheme. J. Am. Chem. Soc., 2024, Accepted.DOI: 10.1021/jacs.4c11827https://doi.org/10.1021/jacs.4c11827 原位XPS、原位XRD、原位Raman、原位FTIR