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Platinum Group Metal Catalyst (RuOx, PtOx, and IrOx)-Decorated Ceria-Zirconia Solid Solution as High Active Oxygen Carriers for Solar Thermochemical CO2 Splitting
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-06-14 , DOI: 10.1021/acscatal.2c02044
Zhenpan Chen 1, 2, 3 , Qingqing Jiang 2, 4 , Hongyu An 2 , Juan Zhang 2 , Shuoqi Hao 1 , Xinju Li 1 , Lili Cai 2 , Wenguang Yu 2 , Kuiyi You 1, 3 , Xuefeng Zhu 2 , Can Li 2
Affiliation  

Ceria substituted with zirconium (Ce1–xZrxO2) is a promising material in two-step thermochemical CO2/H2O splitting cycles due to its great oxygen storage capacity and potential fuel production. However, the Ce1–xZrxO2 solid solution exhibits a relatively slower fuel release rate than cerium oxide alone. Herein, in order to improve the solar-to-fuel energy conversion efficiency, noble metal catalysts (RuOx, PtOx, and IrOx) are used to boost the CO release rate of Ce0.85Zr0.15O2 (CZ15)-based two-step thermochemical CO2 splitting. Compared with intrinsic Ce0.85Zr0.15O2, the maximal CO release rate can be increased by 35% after loading 0.4 atom % IrOx as a catalyst on the surface of Ce0.85Zr0.15O2. Interestingly, the initial CO release rate can be increased by three times when a small amount of IrOx (1.0 atom %) is doped into the crystal structure of Ce0.85Zr0.15O2 through a solution combustion method. This catalytic effect is ascribed to the increased mixed ionic and electric conductivity within the ceramic bulk and the enhanced chemical reaction rate at the gas–solid interface for iridium-decorated ceria-zirconia solid solution. Our work demonstrates that interface engineering and bulk modification through adding the selected catalyst can effectively enhance the CO2 splitting rate of Ce1–xZrxO2 oxygen carriers, which provides a promising strategy to promote the fuel release rates of other kinetics-restricted thermochemical CO2/H2O splitting cycles.

中文翻译:

铂族金属催化剂(RuOx、PtOx 和 IrOx)-修饰的氧化铈-氧化锆固溶体作为太阳能热化学 CO2 分解的高活性氧载体

锆取代的二氧化铈(Ce 1– x Zr x O 2 )由于其巨大的储氧能力和潜在的燃料生产潜力,在两步热化学CO 2 /H 2 O 分解循环中是一种很有前途的材料。然而,Ce 1- x Zr x O 2固溶体表现出比单独的氧化铈相对较慢的燃料释放速率。在此,为了提高太阳能到燃料的能量转换效率,使用贵金属催化剂(RuO x、PtO x和 IrO x)来提高 Ce 0.85 Zr 0.15 O的 CO 释放率基于2 (CZ15) 的两步热化学 CO 2分解。与本征Ce 0.85 Zr 0.15 O 2相比,在Ce 0.85 Zr 0.15 O 2表面负载0.4 atom % IrO x作为催化剂后,最大CO释放率可提高35% 。有趣的是,当在 Ce 0.85 Zr 0.15 O 2的晶体结构中掺杂少量 IrO x (1.0 atom %) 时,初始 CO 释放速率可提高 3 倍。通过溶液燃烧法。这种催化作用归因于陶瓷块内混合离子和电导率的增加以及铱修饰的二氧化锆-氧化锆固溶体气固界面处化学反应速率的提高。我们的工作表明,通过添加选定的催化剂进行界面工程和本体改性可以有效提高Ce 1- x Zr x O 2氧载体的CO 2分解速率,这为提高其他动力学限制的燃料释放速率提供了一种有前景的策略。热化学 CO 2 /H 2 O 分裂循环。
更新日期:2022-06-14
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