南湖新闻网讯(通讯员 邹思榕)近日,我校理学院陈浩教授带领的先进材料与绿色催化科研团队在Nature Communications发表题为“Designing reliable and accurate isotope tracer experiments for CO2photoreduction”的研究论文,该研究针对目前人工光合作用CO2还原反应同位素溯源标准方法缺失,提出了CO2还原反应中同位素示踪实验的标准指南。
二氧化碳(CO2)通过人工光合作用生成可再生合成燃料是一种可产生替代能源原料的方法,有望与化石燃料竞争并最终取代化石燃料。然而,由于CO2光还原反应的转化效率很低,且存在难以察觉的引入碳污染,因此准确地追踪溯源CO2光还原产物极具挑战性。同位素示踪实验已用于解决这一问题,但由于反应物、产物和催化剂本身的相似性,现有的同位素溯源方法容易产生假阳性结果,很难获得可靠的CO2光还原过程。因此,必须尽快研究制定准确有效的策略来评估CO2光还原领域内各种潜在的CO2光还原产物。
鉴于此,我校理学院先进材料与绿色催化团队通过实验,首次证明了当前人工光合作用CO2光还原同位素示踪实验方法存在的不足,利用标准同位素标记分子和GC-MS仪器分析的基本原理,揭示了同位素示踪研究中经常被忽视的假阳性现象。进一步,通过制定严格的CO2光还原同位素溯源策略来消除假阳性结果。通过广泛的测试,系统地提出了CO、烷烃、醇、羧酸和烯烃等各种CO2还原潜在产物的标准光谱同位素示踪实验方法。开创性的设计使用双GC色谱柱并联方案策略实现了上述潜在产物的同时分析,并针对多种已报道的CO2光还原体系对建立的新方案进行了验证。这项研究建立了科学的人工光合作用CO2光还原溯源的检测方法,并制定了严格的检测标准程序,这一研究将帮助研究人员规避同位素示踪实验中的陷阱和错误,为研究人员设计更高效的光催化剂提供更严谨的检测标准,有助于研究人员更准确的理解和分析CO2光还原反应。
近来,我校理学院陈浩教授带领的先进材料与绿色催化科研团队与国内外相关科研团队展开合作,在《自然通讯》(Nat. Commun., 2023, 14, 2534.; Nat. Commun., 2023, 14, 2473.)、《先进材料》(Adv. Mater., 2023, 35, 2302538.)、《先进功能材料》(Adv. Funct. Mater., 2023, 33, 2303335.) 等国际期刊发表了关于人工光合作用CO2还原领域的系列研究成果,为减污降碳工作提供了有力科技支撑。
【英文摘要】
The photoreduction of carbon dioxide (CO2) into renewable synthetic fuels is an attractive approach for generating alternative energy feedstocks that may compete with and eventually displace fossil fuels. However, it is challenging to accurately trace the products of CO2photoreduction on account of the poor conversion efficiency of these reactions and the imperceptible introduced carbon contamination. Isotope-tracing experiments have been used to solve this problem, but they frequently yield false-positive results because of improper experimental execution and, in some cases, insufficient rigor. Thus, it is imperative that accurate and effective strategies for evaluating various potential products of CO2photoreduction are developed for the field. Herein, we experimentally demonstrate that the contemporary approach toward isotope-tracing experiments in CO2photoreduction is not necessarily rigorous. Several examples of where pitfalls and misunderstandings arise, consequently making isotope product traceability difficult, are demonstrated. Further, we develop and describe standard guidelines for isotope-tracing experiments in CO2photoreduction reactions and then verify the procedure using some reported photoreduction systems.
原文链接:
https://www.nature.com/articles/s41467-023-38052-0
https://www.nature.com/articles/s41467-023-37545-2
https://onlinelibrary.wiley.com/doi/10.1002/adma.202302538
https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.202303335
审 核:陈浩