Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination

Ali，Sajjad1,2; Lian，Zan1; Li，Bo1

2021

10.1021/acsanm.1c00945

ACS Applied Nano Materials   影响因子和分区

2574-0970

2574-0970

In this work, supported single Au on graphdiyne is examined as an efficient catalyst for acetylene hydrochlorination. The adsorption of reactants C2H2 and HCl has a paramount influence on the reaction mechanism. It is indicated that C2H2 adsorption is much stronger than the counterpart of HCl for most of the investigated cases. An Eley-Rideal (E-R) mechanism is first investigated, which is initiated with C2H2 adsorption. In the following steps, the adsorbed C2H2 becomes the site to bind and activate HCl, which leads to formation of the product. It is also revealed that single Au experienced a redox cycle along the reaction pathway. The largest barrier is calculated to be 0.57 eV, corresponding to the product desorption. On the other hand, a novel Langmuir-Hinshelwood (L-H)-like mechanism is also reported, which started with coadsorption of HCl and C2H2. It is noted that the barriers of the LH mechanism are smaller than those of the ER mechanism. Moreover, supported single Au on graphdiyne has much improved performance than the counterpart on pristine graphene and single-walled carbon nanotube support. This work clearly demonstrated the superior performance of supported single Au in acetylene hydrochlorination and the potential of novel support graphdiyne in single-atom catalysis.

acetylene hydrochlorination density functional theory graphdiyne reaction mechanism single-atom catalyst

SCI ; EI

英语

其他

National Natural Science Foundation of China[21573255] ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)[U1501501]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000668366800057

AMER CHEMICAL SOC

20212610566926

Acetylene ; Adsorption ; Catalysts ; Chlorine compounds ; Density functional theory ; Lighting ; Redox reactions ; Single-walled carbon nanotubes (SWCN)

Precious Metals:547.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Probability Theory:922.1

2-s2.0-85108619243

Scopus

1.Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang,Liaoning,110016,China
2.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China

Ali，Sajjad,Lian，Zan,Li，Bo. Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination[J]. ACS Applied Nano Materials,2021,4(6):6152-6159.

Ali，Sajjad,Lian，Zan,&Li，Bo.(2021).Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination.ACS Applied Nano Materials,4(6),6152-6159.

Ali，Sajjad,et al."Density Functional Theory Study of a Graphdiyne-Supported Single Au Atom Catalyst for Highly Efficient Acetylene Hydrochlorination".ACS Applied Nano Materials 4.6(2021):6152-6159.