邢金媛,朱梦婷,王婷,李艳明,鲁继青.Pt/MOx(M=Ni,Fe,Co,Ce)催化剂上CO氧化反应中抗H2O与CO2的性能研究[J].分子催化,2019,33(4):309-322 |
Pt/MOx(M=Ni,Fe,Co,Ce)催化剂上CO氧化反应中抗H2O与CO2的性能研究 |
CO Oxidation over Pt/MOx(M=Ni, Fe, Co, Ce) Catalysts and Their Tolerance to CO2 and H2O |
投稿时间:2019-06-25 修订日期:2019-07-23 |
DOI: |
中文关键词: Pt催化剂 CO氧化 抗H2O与抗CO2能力 实际反应条件 动力学 |
英文关键词:Pt catalyst CO oxidation CO2 and H2O tolerant actual reaction conditions kinetics |
基金项目:国家自然科学基金(No.21773212,21643007) |
作者 | 单位 | E-mail | 邢金媛 | 浙江师范大学 物理化学研究所, 先进催化材料教育部重点实验室, 浙江 金华 321004 | | 朱梦婷 | 浙江师范大学 物理化学研究所, 先进催化材料教育部重点实验室, 浙江 金华 321004 | | 王婷 | 浙江师范大学 物理化学研究所, 先进催化材料教育部重点实验室, 浙江 金华 321004 | | 李艳明 | 浙江师范大学 图文信息中心, 浙江省金华市迎宾大道688号, 浙江 金华 321004 | | 鲁继青 | 浙江师范大学 物理化学研究所, 先进催化材料教育部重点实验室, 浙江 金华 321004 | jiqinglu@zjnu.cn |
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中文摘要: |
我们研究了4种负载型Pt催化剂(1Pt/NiO、1Pt/FeOx、1Pt/Co3O4和Pt/CeO2)上不同反应条件下CO氧化活性及抗H2O和CO2性能.发现反应气氛中CO2的加入与CO形成了竞争吸附,并在催化剂表面形成了碳酸盐物种堵塞了活性位,从而导致催化剂失活.反应气氛中H2O的加入对1Pt/CeO2催化剂的活性有所抑制,但对1Pt/FeOx、1Pt/NiO和1Pt/Co3O4催化剂的活性却有促进作用.在1Pt/FeOx和1Pt/CeO2催化剂上的分步反应实验和动力学研究表明,尽管H2O的加入在两种催化剂上均与CO形成了竞争吸附,但在1Pt/FeOx催化剂上H2O在载体表面解离形成的羟基更易与CO反应,开辟了新的反应途径,从而提高了反应性能.此外,H2O的加入能有效分解该催化剂上的碳酸盐物种,从而保持了其稳定性. |
英文摘要: |
Supported Pt catalysts (1Pt/NiO, 1Pt/FeOx, 1Pt/Co3O4 and 1Pt/CeO2) were tested for CO oxidation under different reaction conditions to investigate their resistance to H2O and CO2. It was found that the addition of CO2 resulted in its competitive adsorption with CO and the formation of carbonate species, which blocked the active site and consequently the catalyst deactivation. The addition of H2O inhibited the activity of the Pt/CeO2 catalyst, but promoted those of the 1Pt/FeOx, 1Pt/NiO and 1Pt/Co3O4 catalysts. For the 1Pt/FeOx and 1Pt/CeO2 catalysts, detailed kinetic results and staged reaction indicated thatalthough the addition of H2O brought up competitive adsorption with CO on both catalysts, however, on the 1Pt/FeOx catalyst, the fast reaction between CO and the surface hydroxyl groups formed via H2O dissociation on the support surfaceopened a new reaction way, which thus improved the catalytic performance. In addition, the addition of H2O could effectively decompose the carbonate and sustain the catalyst stability. |
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