Implications of boron doping on electrocatalytic activities of graphyne and graphdiyne families: a first principles study

被引:60
作者
Das, Bikram Kumar [1 ]
Sen, Dipayan [1 ]
Chattopadhyay, K. K. [1 ,2 ]
机构
[1] Jadavpur Univ, Dept Phys, Thin Film & NanoSci Lab, Kolkata 700032, India
[2] Jadavpur Univ, Sch Mat Sci & Nanotechnol, Kolkata 700032, India
关键词
OXYGEN REDUCTION REACTION; METAL-FREE ELECTROCATALYSTS; TOTAL-ENERGY CALCULATIONS; FUEL-CELLS; DOPED GRAPHENE; CARBON; CATALYST; DEHYDROBENZOANNULENES; TRANSITION; MECHANISM;
D O I
10.1039/c5cp05768j
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
Dispersive force corrected density functional theory is used to map the oxygen reduction reaction (ORR) kinetics of six kinds of graphyne (Gy) and graphdiyne (Gdy) systems (namely alpha Gy, beta Gy, gamma Gy, delta Gy, 6,6,12Gy, RGy and Gdy) with substitutional boron (B) atom doping. To this end, the most favorable sites for B doping of each structures are determined by comparing their formation energies and then the best configuration for di-oxygen (O-2) adsorption is computed by analyzing the corresponding adsorption energies. Even though oxygen adsorption is found to be energetically favorable on all of these and all Gys and Gdy are found to distinctly favor the four electron pathways for ORR, a reaction scheme with monotonically exothermic Delta G is observed only for B doped RGy. Further computations performed by varying electrode potential indicated this monotonically exothermic nature of the Delta G of B doped RGy to persist in the range 0-0.22 V and also indicated the first (H+ + e) transfer step to be the rate limiting step.
引用
收藏
页码:2949 / 2958
页数:10
相关论文
共 54 条
[1]   Theory at the electrochemical interface: reversible potentials and potential-dependent activation energies [J].
Anderson, AB .
ELECTROCHIMICA ACTA, 2003, 48 (25-26) :3743-3749
[2]   A QUANTUM-THEORY OF MOLECULAR-STRUCTURE AND ITS APPLICATIONS [J].
BADER, RFW .
CHEMICAL REVIEWS, 1991, 91 (05) :893-928
[3]   STRUCTURE-PROPERTY PREDICTIONS FOR NEW PLANAR FORMS OF CARBON - LAYERED PHASES CONTAINING SP2 AND SP ATOMS [J].
BAUGHMAN, RH ;
ECKHARDT, H ;
KERTESZ, M .
JOURNAL OF CHEMICAL PHYSICS, 1987, 87 (11) :6687-6699
[4]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[5]  
Carrette L, 2001, FUEL CELLS, V1, P5, DOI 10.1002/1615-6854(200105)1:1<5::AID-FUCE5>3.0.CO
[6]  
2-G
[7]   High resolution mapping of oxygen reduction reaction kinetics at polycrystalline platinum electrodes [J].
Chen, Chang-Hui ;
Meadows, Katherine E. ;
Cuharuc, Anatolii ;
Lai, Stanley C. S. ;
Unwin, Patrick R. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (34) :18545-18552
[8]   Why Do Boron and Nitrogen Doped α- and γ-Graphyne Exhibit Different Oxygen Reduction Mechanism? A First-Principles Study [J].
Chen, Xin ;
Qiao, Qingan ;
An, Li ;
Xia, Dingguo .
JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (21) :11493-11498
[9]   Metal-free doped carbon materials as electrocatalysts for the oxygen reduction reaction [J].
Daems, Nick ;
Sheng, Xia ;
Vankelecom, Ivo F. J. ;
Pescarmona, Paolo P. .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (12) :4085-4110
[10]   Platinum-graphene hybrid nanostructure as anode and cathode electrocatalysts in proton exchange membrane fuel cells [J].
Divya, P. ;
Ramaprabhu, S. .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (14) :4912-4918