CIESC Journal ›› 2020, Vol. 71 ›› Issue (10): 4820-4825.doi: 10.11949/0438-1157.20200714

• Material science and engineering, nanotechnology • Previous Articles     Next Articles

Theoretical study on electrocatalytic nitrogen fixation performance of two-dimensional AuP2

Xiaorong ZHU(),Yafei LI()   

  1. School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, Jiangsu, China
  • Received:2020-06-05 Revised:2020-07-24 Online:2020-10-05 Published:2020-08-10
  • Contact: Yafei LI E-mail:xiaorongzhu_njnu@163.com;liyafei@njnu.edu.cn

Abstract:

The electrochemical conversion of nitrogen (N2) and water (H2O) into ammonia (NH3) under normal temperature and pressure conditions is a green and environmentally friendly method of ammonia synthesis. However, because N2 has a very high chemical inertness, an electrocatalyst must be used to accelerate the kinetic process of the reaction. In this paper, we use density functional theory calculations to reveal that AuP2, a new type of two-dimensional inorganic material, has good catalytic activity for the electrochemical reduction of N2 to NH3. In the two-dimensional AuP2 material, significant charge transfer occurs between Au and P atoms due to the difference in electronegativity, so that positively charged P can be used as an active site to promote nitrogen reduction. Our calculations show that the rate-determining step of the entire reaction is the process of generating *NNH from N2 with a limiting voltage of 1.2 V, and the catalytic activity can be comparable to some metal catalysts. This work provides new ideas for the design of high-efficiency nitrogen reduction electrocatalysts.

Key words: two-dimensional materials, AuP2, electrocatalysis, nitrogen reduction reaction, density functional theory calculations

CLC Number: 

  • O 643.36

Fig.1

Top (a) and side (b) views of two-dimensional (2D) AuP2"

Fig.2

Phonon spectrum (a) and the results of MD simulations (b) of 2D AuP2"

Fig.3

Band structure (a) and density of states (DOS) (b) of 2D AuP2"

Fig.4

Views of intermediates [(a)—(e)] and free energy diagrams (f) of NRR on 2D AuP2"

Fig.5

Total density of state of two-dimensional AuP2 and partial density of state of different orbitals in Ⅰ type P"

1 Deng J, Iñiguez J A, Liu C. Electrocatalytic nitrogen reduction at low temperature[J]. Joule, 2012, 2(5): 846-856.
2 Rosca V, Duca M, de Groot M T, et al. Nitrogen cycle electrocatalysis[J]. Chemical Reviews, 2009, 109(6):2209-2244.
3 Shipman M A, Symes M D. Recent progress towards the electrosynthesis of ammonia from sustainable resources[J]. Catalysis Today, 2017, 286: 57-68.
4 Foster S L, Bakovic S I P, Duda R D, et al. Catalysts for nitrogen reduction to ammonia[J]. Nature Catalysis, 2018, 1(7): 490-500.
5 Suryanto B H R, Du H L, Wang D B, et al. Challenges and prospects in the catalysis of electroreduction of nitrogen to ammonia[J]. Nature Catalysis, 2019, 2(4): 290-296.
6 Guo C X, Ran J R, Vasileff A, et al. Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions[J]. Energy and Environmental Science, 2018, 11(1): 45-56.
7 Jia H P, Quadrelli E A. Mechanistic aspects of dinitrogen cleavage and hydrogenation to produce ammonia in catalysis and organometallic chemistry: relevance of metal hydride bonds and dihydrogen[J]. Chemical Society Reviews, 2014, 43(2): 547-564.
8 Egill S, Thomas B, Sigrídur G, et al. A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction[J]. Physical Chemistry Chemical Physics, 2011, 14(3): 1235-1245.
9 Wang Y, Li Y F. PtTe monolayer: two-dimensional electrocatalyst with high basal plane activity toward oxygen reduction reaction[J]. Journal of the American Chemical Society, 2018, 40(140): 12732-12735
10 Deng D H, Novoselov K S, Fu Q, et al. Catalysis with two-dimensional materials and their heterostructures[J]. Nature Nanotechnology, 2016, 11(3): 218-230.
11 Sun Y F, Gao S, Lei F C, et al. Atomically-thin two-dimensional sheets for understanding active sites in catalysis[J]. Chemical Society Reviews, 2015, 44(3): 623-636.
12 Hong X, Chan K, Tsai C, et al. How doped MoS2 breaks transition-metal scaling relations for CO2 electrochemical reduction[J]. ACS Catalysis, 2016, 6(7): 4428-4437.
13 Chou S S, Sai N, Lu P, et al. Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide[J]. Nature Communications, 2015, 6(10): 8311-8311.
14 Gong Q F, Ding P, Xu M Q, et al. Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction[J]. Nature Communications, 2019, 10(1): 2807.
15 Li L Q, Tang C, Xia B Q, et al. Two-dimensional mosaic bismuth nanosheets for highly selective ambient electrocatalytic nitrogen reduction[J]. ACS Catalysis, 2019, 9(4): 2902-2908.
16 Li X H, Li T S, Ma Y J, et al. Boosted electrocatalytic N2 reduction to NH3 by defect‐rich MoS2 nanoflower[J]. Advanced Energy Materials, 2018, 8(30):1801357.
17 Shi M M, Bao D, Li S J, et al. Anchoring PdCu amorphous nanocluster on graphene for electrochemical reduction of N2 to NH3 under ambient conditions in aqueous solution[J]. Advanced Energy Materials, 2018, 8(21):1800124.
18 Du Y Q, Jiang C, Xia W, et al. Electrocatalytic reduction of N2 and nitrogen-incorporation process on dopant-free defect graphene[J]. Journal of Materials Chemistry A, 2020, 8(1): 55-61.
19 Yu X, Han P, Wei Z, et al. Boron-doped graphene for electrocatalytic N2 reduction[J]. Joule, 2018, 2(8): 1610-1622.
20 He T W, Matta S K, Du A, et al. Single tungsten atom supported on N-doped graphyne as a high-performance electrocatalyst for nitrogen fixation under ambient conditions[J]. Physical Chemistry Chemical Physics, 2019, 21(3): 1546-1551.
21 Zhao J X, Chen Z F. Single Mo atom supported on defective boron nitride monolayer as an efficient electrocatalyst for nitrogen fixation: a computational study[J]. Journal of the American Chemical Society, 2017, 139(36): 12480-12487.
22 Abel M, Clair S, Ourdjini O, et al. Single layer of polymeric Fe-phthalocyanine: an organometallic sheet on metal and thin insulating film[J]. Journal of the American Chemical Society, 2011, 133(5): 1203-1205.
23 Kambe T, Sakamoto R, Hoshiko K, et al. π-conjugated nickel bis(dithiolene) complex nanosheet[J]. Journal of the American Chemical Society, 2013, 135(7): 2462-2465.
24 Song Q L, Jiang S, Hasell T, et al. Porous organic cage thin films and molecular-sieving membranes[J]. Advanced Materials, 2016, 28(13):2629-2637.
25 Xu G Y, Nie P, Dou H, et al. Exploring metal organic frameworks for energy storage in batteries and supercapacitors[J]. Materials Today, 2017, 20(4): 191-209.
26 Wu S, Min H, Shi W, et al. Multicenter metal–organic framework‐based ratiometric fluorescent sensors[J]. Advanced Materials, 2020, 32(3):1805871.
27 Zhu L, Liu X, Jiang H, et al. Metal–organic frameworks for heterogeneous basic catalysis[J]. Chemical Reviews, 2017, 117(12): 8129-8176.
28 Tian H, Zhang J Q, Ho W K, et al. Two-dimensional metal-phosphorus network[J]. Matter, 2020, 2(1):111-118.
29 Kresse G, Furthmüller J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set[J]. Physical Review B, 1996, 54(16):11169-11186.
30 Blöchl P E. Projector augmented-wave method[J]. Physical Review B, 1994, 50(24):17953-17979.
31 Perdew J P, Burke K, Ernzerhof M. Generalized gradient approximation made simple[J]. Physical Review Letters, 1996, 77(18): 3865-3868.
32 Baroni S, de Gironcoli S, Dal Corso A, et al. Phonons and related crystal properties from density-functional perturbation theory[J]. Reviews of Modern Physics, 2001, 73(2): 515-562.
33 Nørskov J K, Rossmeisl J, Logadottir A A, et al. Origin of the overpotential for oxygen reduction at a fuel-cell cathode[J]. Journal of Physical Chemistry B, 2004, 108(46): 17886-17892.
34 Grimme S. Semiempirical GGA-type density functional constructed with a long‐range dispersion correction[J]. Journal of Computational Chemistry, 2006, 27(15): 1787-1799.
35 Mathew K, Sundararaman R, Letchworthweaver K, et al. Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways[J]. Journal of Chemical Physics, 2014, 140(8): 084106.
36 Montoya J H, Tsai C, Vojvodic A, et al. The challenge of electrochemical ammonia synthesis: a new perspective on the role of nitrogen scaling relations[J]. ChemSusChem, 2015, 8(13): 2180-2186.
[1] Jing XU, Zixuan YOU, Junqi ZHANG, Zheng CHEN, Deguang WU, Feng LI, Hao SONG. Advances in engineering electroactive biofilms by synthetic biology approaches [J]. CIESC Journal, 2020, 71(9): 3950-3962.
[2] Qi ZHOU, Honglei DING, Detong GUO, Weiguo PAN, Wei DU. Recent advances in catalytic methods of CO2 hydrogenation to clean energy [J]. CIESC Journal, 2020, 71(8): 3428-3443.
[3] Tong YANG, Xiaobo HE, Fengxiang YIN. Preparation of M-MOF-74 (M = Ni, Co, Zn) and its performance in electrocatalytic synthesis of ammonia [J]. CIESC Journal, 2020, 71(6): 2857-2870.
[4] Muyun ZHENG, Yuchi WAN, Ruitao LYU. Research progress on electrocatalytic nitrogen reduction reaction catalysts for ammonia synthesis [J]. CIESC Journal, 2020, 71(6): 2481-2491.
[5] Xidong LIN, Youchen TANG, Quanfei SU, Shaohong LIU, Dingcai WU. Hierarchical porous carbon materials: structure design, functional modification and new energy devices applications [J]. CIESC Journal, 2020, 71(6): 2586-2598.
[6] Yanqi LIU, Ludong HE, Peichao LIAN, Xinzhi CHEN, Yi MEI. Progress on stability enhancement of black phosphorene [J]. CIESC Journal, 2020, 71(3): 936-944.
[7] LIU Changjian1,LI Debao2,YANG Shicheng3,LI Weibin3,HU Sheng3,ZHANG Zhihua3. Integrated process of electrochemical hydrogengation and electrooxidation of diesel oil [J]. CIESC Journal, 2012, 63(1): 198-202.
[8] XU Mai,WANG Fengwu,HU Yunhu,FANG Wenyan,ZHU Chuangao. Investigation on the electrocatalytic degradation of methyl orange on Ti/nanoTiO2-PAn electrode [J]. , 2011, 30(11): 2554-.
[9] DIAO Zenghui,LI Mingyu,SONG Lin,ZENG Fanyin,WANG Xinle. Degradation of Crystal violet with a novel photo-electro-chemical
catalytic method
[J]. , 2010, 29(6): 1148-.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed   
[1] HE Liang, ZHANG Shufen, TANG Bingtao, WANG Lili, YANG Jinzong. Dyeability of Polylactide Fabric with Hydrophobic Anthraquinone Dyes[J]. , 2009, 17(1): 156 -159 .
[2] ZHAO Suying, HUANG Jingzhao, WANG Liang'en, HUANG Guoqiang. Coupled Reaction/Distillation Process for Hydrolysis of Methyl Acetate[J]. , 2010, 18(5): 755 -760 .
[3] Gao Yonggui, Yao Shanjing and Yang Xianqiang (Department of Chemical and Biochemical Engineering, Department of Tea Science, Zhejiang University, Hangzhou 310027). EFFECT OF FREE RADICALS ON INTACT CELL MEMBRANE FLUIDITY BY DPH LABELED[J]. , 2000, 51(S1): 182 -185 .
[4] CAO Xiangsheng, FU Kunming, QIAN Dong, ZHU Zhaoliang, MENG Xuezheng. Effect of C/N ratio on nitrite accumulation in dentrifying process with methanol as carbon source[J]. CIESC Journal, 2010, 61(11): 2939 -2943 .
[5] . [J]. , 2001, 52(7): 658 .
[6] FENG Xiangchun.

STATISTICAL ANALYSIS ON AUTHORS IN JOURNAL OF CHEMICAL INDUSTRY AND ENGINEERING(1998~2002)

[J]. , 2004, 55(11): 1925 -1927 .
[7] Chen Shu, Yu Qiquan, Jin Yun, Pan Li, Lin Po, Zhang Quide, Song Wen and Zhang Suhua Chemistry Department of Beijing University. Kinetics of Oxidative Dehydrogenation of Butene-2 on Multicomponent Molybdates Catalyst[J]. , 1982, 33(1): 35 -49 .
[8] YU Xiaojiao;YAO Binghua;ZHOU Xiaode.

TREATMENT OF Cr(Ⅲ) WASTE-WATER WITH EMULSION LIQUID MEMBRANE

[J]. , 2004, 55(10): 1736 -1739 .
[9] Kang Dingxue, Chen Xianman, Liu Ziqin, Wang Fengming Xing Yufang, Xiao Fuquan and Li Pincui Qinghai Institute of Salt Lake, Academia Sinica. Extraction of Potassium, Rubidium and Cesium in Brine with Clinoptilolite Rock[J]. , 1983, 34(2): 173 -183 .
[10] ZHANG Zhanwen;LI Bo;TANG Yongjian;CHEN Sufen;FENG Jianhong;
WANG Chaoyang;WEI Sheng;YUAN Yuping
. Filling hollow PS-PVA-CH microspheres with deuterium[J]. , 2007, 58(10): 2647 -2651 .