Thin-sheet microfibrous-structured Pd-MgO-Al2O3/Al-fiber catalysts were developed for high-throughput catalytic methane combustion with 3-15 vol% water vapor in feed gas. The catalysts were obtained by hydrothermally growing Mg-Al mixed-oxide precursors (e.g., layered double hydroxides (LDHs) plus MgCO3) on Al-fiber surfaces followed by placing 0.5 wt% Pd on the as-obtained substrates by impregnation. Transformation of Pd/MgAl-LDH-MgCO3 mounted on the Al-fiber into Pd-MgO-Al2O3 via in situ reaction activation markedly enhances the catalyst basicity and electron density of metallic Pd, thus weakening support electrophilicity and stabilizing PdO against the formation of inactive Pd4+ species. This preferred catalyst with high intrinsic activity (turnover frequency 135 h(-1) at 290 degrees C and 3 vol% water vapor) achieves a very low Ea of only 57 kJ mol(-1), a third that (170 kJ mol(-1)) for the Pd/AlOOH/Al-fiber. This catalyst can stably run for feed gases of 1 vol% methane and 3-15 vol% water vapor in air. (C) 2020 Elsevier Inc. All rights reserved.
机构:
Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
Basile, F.
;
Benito, P.
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Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
Benito, P.
;
Fornasari, G.
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Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
机构:
East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Chai, Ruijuan
;
Li, Yakun
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Li, Yakun
;
Zhang, Qiaofei
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhang, Qiaofei
;
Fan, Songyu
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Fan, Songyu
;
Zhang, Zhiqiang
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhang, Zhiqiang
;
Chen, Pengjing
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Chen, Pengjing
;
Zhao, Guofeng
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhao, Guofeng
;
Liu, Ye
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Liu, Ye
;
Lu, Yong
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
机构:
Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Chen, Chen
;
Yeh, Yu-Hao
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Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Yeh, Yu-Hao
;
Cargnello, Matteo
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Univ Penn, Dept Chem, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Cargnello, Matteo
;
Murray, Christopher B.
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Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
Univ Penn, Dept Mat Sci & Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
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Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
Basile, F.
;
Benito, P.
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Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
Benito, P.
;
Fornasari, G.
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Univ Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, ItalyUniv Bologna, Dipartimento Chim Ind & Mat, ALMA MATER STUDIORUM, I-40136 Bologna, Italy
机构:
East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Chai, Ruijuan
;
Li, Yakun
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Li, Yakun
;
Zhang, Qiaofei
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhang, Qiaofei
;
Fan, Songyu
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Fan, Songyu
;
Zhang, Zhiqiang
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhang, Zhiqiang
;
Chen, Pengjing
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Chen, Pengjing
;
Zhao, Guofeng
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Zhao, Guofeng
;
Liu, Ye
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
Liu, Ye
;
Lu, Yong
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East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R ChinaEast China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 00062, Peoples R China
机构:
Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Chen, Chen
;
Yeh, Yu-Hao
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机构:
Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Yeh, Yu-Hao
;
Cargnello, Matteo
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机构:
Univ Penn, Dept Chem, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
Cargnello, Matteo
;
Murray, Christopher B.
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机构:
Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
Univ Penn, Dept Mat Sci & Engn, Philadelphia, PA 19104 USAUniv Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA