Highly Dispersed Platinum Atoms on the Surface of AuCu Metallic Aerogels for Enabling H2O2 Production

被引:40
作者
Shi, Qiurong [1 ]
Zhu, Wenlei [1 ]
Zhong, Hong [1 ]
Zhu, Chengzhou [1 ]
Tian, Hangyu [1 ]
Li, Jincheng [1 ]
Xu, Mingjie [2 ]
Su, Dong [3 ]
Li, Xing [3 ]
Liu, Dong [1 ]
Xu, Bo Z. [4 ]
Beckman, Scott P. [1 ]
Du, Dan [1 ]
Lin, Yuehe [1 ]
机构
[1] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA
[2] Univ Calif Irvine, Dept Mat Sci & Engn, Irvine, CA 92697 USA
[3] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
[4] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
关键词
atomically dispersed atoms; metallic aerogels; H2O2 selectivity and production; oxygen reduction reaction; density functional theory; OXYGEN-REDUCTION REACTION; FORMIC-ACID; NANOPARTICLES; CATALYSIS; NANORODS; DESIGN; SHELL; FILMS; CORE; PD;
D O I
10.1021/acsaem.9b01314
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
The electrochemical production of hydrogen peroxide is enjoying increasing attention by endowing a promising alternative to the traditional complex and energy-intensive anthraquinone process. Engineering efficient electrocatalysts with desirable activity, selectivity, and stability toward H2O2 electrocatalysis have achieved great progress yet are still challenging. Currently, atomically dispersed Pt atoms on metal have been evidenced as one of the most efficient candidates for their remarkable catalytic activity and selectivity toward H2O2 production through a two electron transfer path for oxygen reduction reaction. Here, atomically dispersed Pt atoms are successfully anchored on the surface of AuCu ultrathin nanowire aerogels (denoted as AD-Pt@AuCu) through kinetically controlled galvanic replacement reaction. The composition-optimized AD-Pt a@ AuCu-144 behaved in a thermodynamically favorable two electron transfer path rather than four as evidenced by a lower thermodynamical overpotential based on first-principles calculation. The H2O2 selectivity reached 91.8% and achieved a continuous yield of 47.5 mg/L H2O2 in 5 h, owing to its unique atomic configuration and robust 3D porous architecture. The AD-Pt@AuCu-144 catalysts may pave a way for favoring the advances of localized electrochemical production of H2O2.
引用
收藏
页码:7722 / 7727
页数:11
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