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Adjacent Pt Nanoparticles and Sub-nanometer WOxClusters Determine Catalytic Isomerization of C7H16    

文献类型:期刊文献

英文题名:Adjacent Pt Nanoparticles and Sub-nanometer WOxClusters Determine Catalytic Isomerization of C7H16

作者:Zhang, Bin[1,2,3,4];Zhou, Wei[1,2,3];Zhang, Jie[1,2,3];Gao, Zirui[1,2,3];Cheng, Danyang[1,2,3];Tang, Lipeng[1,2,3];Liu, Xingwu[1,2,3];Song, Yueqin[5];Dong, Chunyang[1,2,3];Xu, Yao[1,2,3];Yan, Jie[1,2,3];Peng, Mi[1,2,3];Liu, Huizhen[4];Douthwaite, Mark[6];Wang, Meng[1,2,3];Ma, Ding[1,2,3]

机构:[1]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China;[2]Peking Univ, Coll Engn, Beijing 100871, Peoples R China;[3]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China;[4]Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, CAS Key Lab Colloid & Interface & Thermodynam, Beijing 100190, Peoples R China;[5]East China Univ Sci & Technol, Petr Proc Res Ctr, Shanghai 200237, Peoples R China;[6]Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, Wales

年份:2022

卷号:4

期号:8

起止页码:2639

外文期刊名:CCS CHEMISTRY

收录:WOS:【ESCI(收录号:WOS:000842933300001)】;

基金:This work received financial support from the Natural Science Foundation of China (nos. 21725301, 21932002, 22005007, and 21821004) , the National Key R&D Program of China (no. 2017YFB0602200) , and the Chinese Post-doctoral Science Foundation (no. 8206300246) . B.Z. gratefully acknowledges the support of the BoyaPostdoctoral Fellowship of Peking University (2019- 2020) and the Junior Fellowship of Beijing National Lab-oratory of Molecular Science (BMS Junior Fellow, 2020- 2023) . D.M. acknowledges support from the Tencent Foundation through the XPLORER PRIZE and the support from OSSO state key lab.

语种:英文

外文关键词:WOx monolayers; metal-acid catalysis; proximity; bifunctional catalysis; acid quantification

摘要:Processes for the isomerization of light alkanes have been commercialized; however, the isomerization of paraffins (CnH2n+2, n >= 7) remains a challenge. On mesoporous tungsten-zirconia catalyst supported Pt catalysts (Pt/WZrOx), initial isomerization productivity of 5249 mol(i-C7)/mol(Pt)/h was obtained for n-heptane reforming at 275 degrees C and 5 bar of hydrogen. The catalyst possessed quasi-monolayer and uniformly distributed WOx clusters ( diameter of similar to 0.5 nm), and Pt nanoparticles were preferentially deposited in close vicinity to these WOx sub-nanometer monolayers. The initial productivity over the best Pt/WZrOx catalyst was 18 times higher than that of a corresponding physical mixture (0.8 wt % Pt/ZrO2 + WZrOx), highlighting the significance of intimacy between the Pt and WOx species. The isomerization could not be triggered until the acid density of the catalysts reached a threshold because of the necessity of close proximity between adequate acid sites and adjacent Pt metal sites. Meanwhile, the adjacency increased the metallicity of the supported Pt; thus, enabling easier activation of C-H bonds of C7H16. [GRAPHICS] .

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