Direct H2S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production

被引:51
作者
Lou, Minghe [1 ,2 ]
Bao, Junwei Lucas [3 ,4 ,5 ]
Zhou, Linan [1 ,2 ]
Naidu, Gopal Narmada
Robatjazi, Hossein [1 ,2 ,6 ]
Bayles, Aaron I. [1 ,2 ]
Everitt, Henry O. [7 ,8 ]
Nordlander, Peter [9 ,10 ]
Carter, Emily A. [3 ,4 ]
Halas, Naomi J. [1 ,2 ,7 ]
机构
[1] Rice Univ, Dept Chem, Houston, TX 77005 USA
[2] Rice Univ, Lab Nanophoton, Houston, TX 77005 USA
[3] Princeton Univ, Dept Mech & Aerospace Engn, Princeton, NJ 08544 USA
[4] Princeton Univ, Andlinger Ctr Energy & Environm, Princeton, NJ 08544 USA
[5] Boston Coll, Dept Chem, Chestnut Hill, MA 02467 USA
[6] Syzygy Plasmon Inc, Houston, TX 77054 USA
[7] Rice Univ, Dept Elect & Comp Engn, Houston, TX 77005 USA
[8] US Army DEVCOM Army Res Lab, Houston, TX 77005 USA
[9] Rice Univ, Lab Nanophoton, Dept Elect & Comp Engn, Houston, TX 77005 USA
[10] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA
关键词
CATALYTIC DECOMPOSITION; HOT-CARRIER; SULFIDE; NANOPARTICLES; ADSORPTION; H-2; DISSOCIATION; SURFACE; REDUCTION; RESONANCE;
D O I
10.1021/acsenergylett.2c01755
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Plasmonic metal nanostructures have garnered rapidly increasing interest as heterogeneous photocatalysts, facilitating chemical bond activation and overcoming the high energy demands of conventional thermal catalysis. Here we report the highly efficient plasmonic photocatalysis of the direct decomposition of hydrogen sulfide into hydrogen and sulfur, an alternative to the industrial Claus process. Under visible light illumination and with no external heat source, up to a 20-fold reactivity enhancement compared to thermocatalysis can be observed. The substantially enhanced reactivity can be attributed to plasmon-mediated hot carriers (HCs) that modify the reaction energetics. With a shift in the rate-determining step of the reaction, a new reaction pathway is made possible with a lower apparent reaction barrier. Light-driven one-step decomposition of hydrogen sulfide represents an exciting opportunity for simultaneous high-efficiency hydrogen production and low-temperature sulfur recovery, important in many industrial processes.
引用
收藏
页码:3666 / 3674
页数:9
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