调变 CoO 上生物质的选择性吸附位以用于电合成的 Ir 单原子。
Tuning the Selective Adsorption Site of Biomass on Co O by Ir Single Atoms for Electrosynthesis.
机构信息
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Provincial Hunan Key Laboratory for Graphene Materials and Devices, College of Chemistry and Chemical Engineering, National Supercomputer Centers in Changsha, Hunan University, Changsha, 410082, P. R. China.
College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, Jiangsu, 210023, P. R. China.
出版信息
Adv Mater. 2021 Feb;33(8):e2007056. doi: 10.1002/adma.202007056. Epub 2021 Jan 20.
The electrosynthesis from 5-hydroxymethylfurfural (HMF) is considered a green strategy to achieve biomass-derived high-value chemicals. As the molecular structure of HMF is relatively complicated, understanding the HMF adsorption/catalysis behavior on electrocatalysts is vital for biomass-based electrosynthesis. The electrocatalysis behavior can be modulated by tuning the adsorption energy of the reactive molecules. In this work, the HMF adsorption behavior on spinel oxide, Co O is discovered. Correspondingly, the adsorption energy of HMF on Co O is successfully tuned by decorating with single-atom Ir. It is observed that compared with bare Co O , single-atom-Ir-loaded Co O (Ir-Co O ) can enhance adsorption with the CC groups of HMF. The synergetic adsorption can enhance the overall conversion of HMF on electrocatalysts. With the modulated HMF adsorption, the as-designed Ir-Co O exhibits a record performance (with an onset potential of 1.15 V ) for the electrosynthesis from HMF.
从 5-羟甲基糠醛（HMF）电合成被认为是实现生物质衍生高价值化学品的绿色策略。由于 HMF 的分子结构相对复杂，因此了解 HMF 在电催化剂上的吸附/催化行为对于基于生物质的电合成至关重要。通过调节反应分子的吸附能可以调节电催化行为。在这项工作中，发现了 HMF 在尖晶石氧化物 CoO 上的吸附行为。相应地，通过单原子 Ir 修饰成功地调谐了 HMF 在 CoO 上的吸附能。观察到与纯 CoO 相比，负载单原子 Ir 的 CoO（Ir-CoO）可以增强 HMF 的 CC 基团的吸附。协同吸附可以增强 HMF 在电催化剂上的整体转化。通过调节 HMF 的吸附，所设计的 Ir-CoO 表现出了 HMF 电合成的创纪录性能（起始电位为 1.15V）。
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