Actual reliance of catalytic activities tuned oxygen vacancies on VOx/Ce1-xZrxO2 catalyst for selective oxydehydrogenation of methanol to dimethoxymethane

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL
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Abstract

Metal oxide catalysts like ceria-supported vanadia (VOx/Ce1-xZrxO2) with different Zr contents were prepared by coupling ceria-zirconia solid solution and vanadia. Characterization revealed that the insertion of zirconia into ceria significantly improved catalytic activity due to the generation of more oxygen vacancies and distortion of the composite structure. The oxygen vacancy concentration initially increased with the increase of Zr (x= wt%) and peaked at x=0.7 and then decreased. The reliance of oxygen vacancy concentration in VOx/Ce1-xZrxO2 catalyst on their catalytic activity in methanol oxydehydrogenation was further investigated. Results indicated that oxygen vacancies not only activated oxygen species but also cleaved C–H bonds alongside V5+ active site contained terminal oxygen atoms for cleaving O–H and C–H bonds within the adsorbed methanol. The VOx/Ce0.3Zr0.7O2 exhibited the best catalytic activity with the methanol conversion of 76 % and the dimethoxymethane selectivity of 96 % at 200 ℃ and atmospheric pressure in a fixed-bed reactor.

调整 VOx/Ce1-xZrxO2 催化剂上氧空位的催化活性对甲醇选择性氧脱氢生成二甲氧基甲烷的实际依赖性
通过将铈-氧化锆固溶体和钒钛耦合,制备了不同锆含量的金属氧化物催化剂,如铈支撑的钒钛催化剂(VOx/Ce1-xZrxO2)。表征结果表明,在铈中加入氧化锆后,由于产生了更多的氧空位和复合结构的畸变,催化活性显著提高。氧空位浓度最初随着 Zr(x= wt%)的增加而增加,在 x=0.7 时达到峰值,然后下降。进一步研究了 VOx/Ce1-xZrxO2 催化剂中氧空位浓度对其甲醇氧脱氢催化活性的影响。结果表明,氧空位不仅能激活氧物种,还能裂解 C-H 键,因为 V5+ 活性位点含有末端氧原子,可裂解吸附甲醇中的 O-H 和 C-H 键。VOx/Ce0.3Zr0.7O2 的催化活性最好,在固定床反应器中,200 ℃、常压条件下的甲醇转化率为 76%,二甲氧基甲烷选择性为 96%。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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