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    大连化物所等金属-载体界面结构研究取得新进展
    来源：本站 发布时间：2019-04-01 点击数：844

    近日，中国(guo)科学(xue)院大连化(hua)学(xue)物(wu)理(li)研(yan)(yan)究所(suo)催化(hua)基(ji)础国(guo)家(jia)重点实(shi)验室催化(hua)反应(ying)化(hua)学(xue)研(yan)(yan)究组副研(yan)(yan)究员(yuan)周燕、研(yan)(yan)究员(yuan)申文杰等与德国(guo)卡尔(er)斯鲁厄理(li)工学(xue)院教授(shou)汪跃民、丹麦托普索公司博士Jens Sehested等合作，在(zai)(zai)铜催化(hua)剂活(huo)性位(wei)原(yuan)子结构及反应(ying)机理(li)研(yan)(yan)究方(fang)面取得新(xin)进展。研(yan)(yan)究成果(guo)在(zai)(zai)线(xian)发表在(zai)(zai)《自然-催化(hua)》（）上。

    　　Cu/CeO2催化(hua)剂(ji)在(zai)水气变(bian)换、合(he)成甲醇等(deng)合(he)成气化(hua)学反应中表现(xian)出优异(yi)性能，但对其(qi)活性位原(yuan)子结构(gou)和(he)催化(hua)机理还知(zhi)之甚(shen)少。

    　　该研究团队利用球差较正扫描透射电镜（AC-STEM）和电子能量损失谱（EELS）表征了金属-载体界面原子结构和化学配位环境，发现铜原子簇主要呈现双层结构（bilayers），界面铜原子的空间结构取决于其与氧化铈表层氧空穴之间的相互作用程度。此外，科研人员通过原位红外光谱等确定了铜原子的化学状态及氧化铈表面氧空穴分布；结合DFT计算，描述了界面铜原子向氧化铈电子转移过程及相互作用机制。该工作中，科研人员提出了copper bilayer模型概念，模型的上层为金属态铜原子（Cu0），而下层为一价铜原子（Cu+）。研究还发现水气变换反应的活性位为一价铜原子与邻近的氧化铈表面的氧空穴（Cu+-Ov-Ce3+）：CO在一价铜表面吸附活化，而水分子则在邻近的氧化铈空穴位解离活化。该工作揭示了Cu/CeO2催化(hua)剂(ji)活(huo)性位的原子结构，为通过调控金(jin)属-氧化(hua)物相互作(zuo)用方式研制高活(huo)性催化(hua)剂(ji)提供了实验和(he)理(li)论基础。

    　　该研究得(de)到国家自然科学基金委相关(guan)项目的资助。

     

    大连化物(wu)所等金属-载体界面结构研究(jiu)取得新(xin)进展