Rational design of highly H2O- and CO2-tolerant hydroxyapatite-supported Pd catalyst for low-temperature methane combustion

Rational design of highly H2O- and CO2-tolerant hydroxyapatite-supported Pd catalyst for low-temperature methane combustion
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高耐H2O和CO2的羟基磷灰石负载Pd低温甲烷燃烧催化剂的合理设计

DOI:
10.1016/j.cej.2020.125225
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发表时间:
2020-09
影响因子:
15.1
通讯作者:
Lilong Jiang
Lilong Jiang
中科院分区:
工程技术1区
文献类型:
--
作者:
Yangyu Zhang;Jie Zhu;Shusheng Li;Yihong Xiao;Yingying Zhan;Xiuyun Wang;Chak-tong Au;Lilong Jiang

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首次采用离子交换法和单模微波技术合成了羟基磷灰石(HAP)负载钯(Pd)。研究了离子交换时间对Pd/HAP催化剂甲烷燃烧性能的影响。结果表明,离子交换时间对Pd粒子在HAP上的分散性和粒径有影响。当时间为5 h(表示为Pd/HAP-5)时,催化剂上的T90(90%CH 4转化的温度)为400 °C。当反应时间为20 h时,催化剂的催化性能有所下降。Pd/HAP-5的优异性能归因于(i)丰富的表面PdO和活性氧物种,(ii)高的Pd分散和还原性,(iii)强的CH 4吸附。与传统的Pd基催化剂不同,Pd/HAP-5在5%volCO2存在下表现出改善的性能。此外,Pd/HAP在7vol%H2O存在下是高度耐久的。最后,我们提出了Pd/HAP催化剂上CH 4燃烧的反应机理。
For the first time, palladium (Pd) supported on hydroxyapatite (HAP) was synthesized by integrating ion-exchange method and single-mode microwave technology. The effect of ion-exchange time on the methane (CH4) combustion performance of Pd/HAP was investigated. It was disclosed that the dispersion and size of Pd particles on HAP is affected by ion-exchange time. When the time was 5 h (denoted as Pd/HAP-5), T90(the temperature for 90% CH4conversion) over the catalyst was 400 °C. However, there was decrease of catalytic performance when the time was 20 h. The eminent performance of Pd/HAP-5 is ascribed to (i) ample surface PdO and active oxygen species, (ii) high Pd dispersion and reducibility, and (iii) strong CH4adsorption. Unlike traditional Pd-based catalysts, Pd/HAP-5 shows improved performance in the presence of 5%volCO2. Moreover, Pd/HAP is highly durable in the presence of 7 vol%H2O. Finally, we propose a reaction mechanism of CH4combustion over the Pd/HAP.
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