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Surface plasmon resonance and defects on tungsten oxides synergistically boost high-selective CO2 reduction for ethylene
Applied Materials Today ( IF 8.3 ) Pub Date : 2020-07-03 , DOI: 10.1016/j.apmt.2020.100744
Changhai Lu , Juan Li , Jiahao Yan , Baojun Li , Baibiao Huang , Zaizhu Lou

Photocatalytic CO2 reduction reaction (CO2-RR) driven by solar energy is one expected “green technology” to produce hydrocarbon, however, the high-valuble C2/Cx-compounds converted from CO2 face great challenges. Herein, high-selective ethylene production is achieved via photocatalytic CO2-RR by using plasmonic tungsten oxides as catalyst under solar light irradiation. Tungsten oxides (WO3-x-2) synthesized by using acid-assisted solvothermal method exhibits thin amorphous surface structure with abundant oxygen vacancies and low-valence tungsten ions (26.1 mol% W5+ and 7.1 mol% W4+). Under full-spectrum light irradiation, ethylene generation rate of WO3-x-2 is 61.6 μmol g  1 h  1 (selectivity of 89.3%) and is 20-fold higher than that of WO3-x-0 with thick amorphous surface. The amorphous surface of tungsten oxides with abundant defects is clearly observed by atomic-resolution high-angle annular dark field scanning transmission electronic microscopy (HAADF-STEM). Light-dependent photocatalytic results demonstrate the synergetic effect of oxygen vacancies, plasmonic hot electrons and photothermal heating boosting CO2-RR on tungsten oxide catalysts for ethylene generation. One possible ethylene generation pathway is proposed based on the detected intermediates during CO2-RR. As far as we known, our work is the first report on plasmonic photocatalytic CO2-RR for high-selective ethylene generation.



中文翻译:

表面等离子体共振和氧化钨上的缺陷协同促进乙烯的高选择性CO 2还原

由太阳能驱动的光催化CO 2还原反应(CO 2 -RR)是生产碳氢化合物的一种预期的“绿色技术”,但是,由CO 2转化的高价值C2 / Cx化合物面临巨大挑战。在此,在太阳光照射下,通过使用等离子体激元氧化钨作为催化剂,通过光催化的CO 2 -RR可以实现高选择性的乙烯生产。用酸辅助溶剂热法合成的钨氧化物(WO 3-x -2)呈现出薄的无定形表面结构,具有丰富的氧空位和低价钨离子(26.1 mol%W 5+和7.1 mol%W 4+)。在全光谱光照射下,WO的乙烯生成率3-X -2是61.6微摩尔 -  1个 H ^  -  1(89.3%的选择性),并且是20倍比的WO更高3-x -0与厚的非晶形表面。通过原子分辨率高角度环形暗场扫描透射电子显微镜(HAADF-STEM)可以清楚地观察到具有大量缺陷的氧化钨的非晶态表面。与光有关的光催化结果表明,氧空位,等离激子热电子和光热加热促进CO 2 -RR对生成乙烯的氧化钨催化剂具有协同作用。根据CO 2期间检测到的中间体,提出了一种可能的乙烯生成途径-RR。据我们所知,我们的工作是有关等离子光催化CO 2 -RR用于高选择性乙烯生成的第一份报告。

更新日期:2020-07-03
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