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Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
Nature Communications ( IF 16.6 ) Pub Date : 2020-03-31 , DOI: 10.1038/s41467-020-15445-z
Bingqiao Xie , Roong Jien Wong , Tze Hao Tan , Michael Higham , Emma K. Gibson , Donato Decarolis , June Callison , Kondo-Francois Aguey-Zinsou , Michael Bowker , C. Richard A. Catlow , Jason Scott , Rose Amal

Although photoexcitation has been employed to unlock the low-temperature equilibrium regimes of thermal catalysis, mechanism underlining potential interplay between electron excitations and surface chemical processes remains elusive. Here, we report an associative zinc oxide band-gap excitation and copper plasmonic excitation that can cooperatively promote methanol-production at the copper-zinc oxide interfacial perimeter of copper/zinc oxide/alumina (CZA) catalyst. Conversely, selective excitation of individual components only leads to the promotion of carbon monoxide production. Accompanied by the variation in surface copper oxidation state and local electronic structure of zinc, electrons originating from the zinc oxide excitation and copper plasmonic excitation serve to activate surface adsorbates, catalysing key elementary processes (namely formate conversion and hydrogen molecule activation), thus providing one explanation for the observed photothermal activity. These observations give valuable insights into the key elementary processes occurring on the surface of the CZA catalyst under light-heat dual activation.



中文翻译:

紫外线和可见光的协同光活化可在铜/氧化锌/氧化铝上增强低温甲醇的合成

尽管已采用光激发来解锁热催化的低温平衡机制,但强调电子激发与表面化学过程之间潜在相互作用的机制仍然难以捉摸。在这里,我们报告了一种关联的氧化锌带隙激发和铜等离子体激发,可以协同促进在铜/氧化锌/氧化铝(CZA)催化剂的铜-氧化锌界面周围产生甲醇。相反,单个组分的选择性激发仅导致一氧化碳产生的促进。伴随着表面铜氧化态和锌局部电子结构的变化,源自氧化锌激发和铜等离子体激发的电子可活化表面吸附物,催化关键的基本过程(即甲酸转化和氢分子活化),从而为观察到的光热活性提供了一种解释。这些观察结果提供了对在光热双重活化下CZA催化剂表面发生的关键基本过程的宝贵见解。

更新日期:2020-04-24
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