Black Phosphorus-Graphene Heterostructure-Supported Pd Nanoparticles with Superior Activity and Stability for Ethanol Electro-oxidation

Tong Wu; Yu Ma; Zhibei Qu; Jinchen Fan; Qiaoxia Li; Penghui Shi; Qunjie Xu; Yulin Min

doi:10.1021/acsami.8b20240

Black Phosphorus-Graphene Heterostructure-Supported Pd Nanoparticles with Superior Activity and Stability for Ethanol Electro-oxidation

ACS Appl Mater Interfaces. 2019 Feb 6;11(5):5136-5145. doi: 10.1021/acsami.8b20240. Epub 2019 Jan 28.

Authors

Tong Wu¹, Yu Ma^{2

3}, Zhibei Qu², Jinchen Fan^{1

2

4}, Qiaoxia Li^{1

4}, Penghui Shi^{1

4}, Qunjie Xu^{1

4}, Yulin Min^{1

4}

Affiliations

¹ Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering , Shanghai University of Electric Power , Shanghai 200090 , P. R. China.
² Department of Chemical Engineering and Biointerfaces Institute , University of Michigan , Ann Arbor , Michigan 48109 , United States.
³ School of Physical Science and Technology , Lanzhou University , Lanzhou 730000 , P. R. China.
⁴ Shanghai Institute of Pollution Control and Ecological Security , Shanghai 200092 , P. R. China.

PMID: 30648393
DOI: 10.1021/acsami.8b20240

Abstract

Rational design supporting material for palladium (Pd)-based catalyst can maximize its electrocatalytic performance for ethanol oxidation reaction (EOR) catalyst in alkaline condition. Utilizing the unique two-dimensional structures and outstanding physicochemical property of graphene and black phosphorus (BP), herein, we proposed and designed a black phosphorus-graphene heterostructure for supporting Pd nanoparticles. Through merely ball-milling of activated graphene (AG) and black phosphorus (BP), the AG-BP hybrid with a linkage of P-C bonding is used as supports of Pd. The obtained Pd/AG-BP hybrid exhibits ultrahigh electrochemical activity toward EOR. Remarkably, it can achieve a high mass peak current density of ∼6004.53 and ∼712.03 mA mg_Pd^-1 before and after the durability tests of 20 000s on EOR, which are ∼7.19 and 80 times higher than those of commercial Pd/C. The experimental analysis and density-functional-theory calculation show that Pd becomes more positive with electrons transfer from Pd to AG-BP supports and is liable to absorb the OH radicals for removing CO_ads intermediate to release active sites on EOR, together with the excellent ability to generate additional OH militants after combining with the AG-BP heterostructure.

Keywords: black phosphorus; catalysts; ethanol electro-oxidation; graphene; palladium.