Defect Engineering of Graphene Hybrid Catalysts for Oxygen Reduction Reactions

doi:10.15541/jim20210197

Abstract

Abstract: Oxygen reduction reaction (ORR) is important for energy and catalytic applications. Therefore, it is significant to develop highly active and selective catalysts to promote ORR. According to the reaction process, ORR can be categorized into two- and four-electrons transfer pathways. In this work, chemically modified graphene sheets with different defects were used as precursors, which were integrated with Ag-7,7,8,8-tetracyanoquinodimethane (Ag-TCNQ) to form hybrid catalysts. The ORR activities of Ag-TCNQ/high defect graphene and Ag-TCNQ/low defect graphene were compared. The results show that the electron transfer number of ORR with Ag-TCNQ/high defect graphene is 2.4. And its corresponding production yield of H₂O₂ is 0.62 mg/h, and Faraday efficiency is 64.45%. In comparison, the electron transfer number of ORR with Ag-TCNQ/low defect graphene is 3.7 and the corresponding half-wave potential is about 0.7 V (vs. RHE). Therefore, high structural defects promote the two-electron process of ORR, while low structural defects facilitate the four-electron process of ORR. In the composites, Ag-TCNQ nanoparticles and graphene have formed a hybrid effect to improve the catalytic activities.

Key words: graphene, defect engineering, Ag-7,7,8,8-tetracyanoquinodimethane, oxygen reduction reaction

CLC Number:

O646

JIANG Lili, XU Shuaishuai, XIA Baokai, CHEN Sheng, ZHU Junwu. Defect Engineering of Graphene Hybrid Catalysts for Oxygen Reduction Reactions[J]. Journal of Inorganic Materials, 2022, 37(2): 215-222.

References

[1] BARACK O.The irreversible momentum of clean energy.Science, 2017, 355: 126-131.
[2] CHU S, MAJUMDAR A.Opportunities and challenges for a sustainable energy future.Nature, 2012, 488(7411): 294-303.
[3] ZHOU R, ZHENG Y, JARONIEC M, et al. Determination of the electron transfer number for the oxygen reduction reaction: from theory to experiment. ACS Catalysis, 2016, 6(7): 4720-4728.
[4] ZHOU W, RAJIC L, CHEN L, et al. Activated carbon as effective cathode material in iron-free electro-Fenton process: integrated H₂O₂ electrogeneration, activation, and pollutants adsorption. Electrochim Acta, 2019, 296: 317-326.
[5] SUN Y, SILVIOLI L, SAHRAIE N R, et al. Activity-selectivity trends in the electrochemical production of hydrogen peroxide over single-site metal-nitrogen-carbon catalysts. Journal of the American Chemical Society, 2019, 141(31): 12372-12381.
[6] WANG C, ZHAO H, WANG J, et al. Atomic Fe hetero-layered coordination between g-C₃N₄ and graphene nanomeshes enhances the ORR electrocatalytic performance of zinc-air batteries. Journal of Materials Chemistry A, 2019, 7(4): 1451-1458.
[7] WANG J, KONG H, ZHANG J, et al. Carbon-based electrocatalysts for sustainable energy applications. Progress in Materials Science, 2021, 116(17): 100717-100754.
[8] YANG L, SHUI J, DU L, et al. Carbon-based metal-free ORR electrocatalysts for fuel cells: past, present, and future. Advanced Materials, 2019, 31(13): e1804799.
[9] LI Y, LU J.Metal-air batteries: will they be the future electrochemical energy storage device of choice.ACS Energy Letters, 2017, 2(6): 1370-1377.
[10] ZHOU M, WANG H L, GUO S.Towards high-efficiency nanoelectrocatalysts for oxygen reduction through engineering advanced carbon nanomaterials.Chemical Society Reviews, 2016, 45(5): 1273-1307.
[11] YANG S, VERDAGUER-CASADEVALL A, ARNARSON L, et al. Toward the decentralized electrochemical production of H₂O₂: a focus on the catalysis. ACS Catalysis, 2018, 8(5): 4064-4081.
[12] QIANG Z, CHANG J H, HUANG C P.Electrochemical generation of hydrogen peroxide from dissolved oxygen in acidic solutions.Water Research, 2002, 36: 85-95.
[13] CAMPOS-MARTIN J M, BLANCO-BRIEVA G, FIERRO J L G. Hydrogen peroxide synthesis: an outlook beyond the anthraquinone process.Angewandte Chemie International Edtion, 2006, 45(42): 6962-6984.
[14] EDWARDS J K, FREAKLEY S J, LEWIS R J, et al. Advances in the direct synthesis of hydrogen peroxide from hydrogen and oxygen. Catalysis Today, 2015, 248(7): 3-9.
[15] RUSSO V, TESSER R, SANTACESARIA E, et al. Chemical and technical aspects of propene oxide production via hydrogen peroxide (HPPO process). Industrial & Engineering Chemistry Research, 2013, 52(3): 1168-1178.
[16] LUO M, YANG Y, GUO S.Precious metal nanocrystals for renewable energy electrocatalysis: structural design and controlled synthesis.Dalton Transaction, 2020, 49(2): 267-273.
[17] ASEFA T.Metal-free and noble metal-free heteroatom-doped nanostructured carbons as prospective sustainable electrocatalysts.Accounts of Chemical Research, 2016, 49(9): 1873-1883.
[18] CHEN Y, JI S, CHEN C, et al. Single-atom catalysts: synthetic strategies and electrochemical applications. Joule, 2018, 2(7): 1242-1264.
[19] ZHU Y P, GUO C, ZHENG Y, et al. Surface and interface engineering of noble-metal-free electrocatalysts for efficient energy conversion processes. Accounts of Chemical research, 2017, 50(4): 915-923.
[20] TANG C, WANG H F, CHEN X, et al. Topological defects in metal-free nanocarbon for oxygen electrocatalysis. Advanced Materials, 2016, 28(32): 6845-6851.
[21] JIA Y, CHEN J, YAO X.Defect electrocatalytic mechanism: concept, topological structure and perspective.Materials Chemistry Frontiers, 2018, 2(7): 1250-1268.
[22] YAN X, JIA Y, YAO X.Defects on carbons for electrocatalytic oxygen reduction.Chemical Society Reviews, 2018, 47(20): 7628-7658.
[23] DORRI MOGHADAM A, OMRANI E, MENEZES P L, et al. Mechanical and tribological properties of self-lubricating metal matrix nanocomposites reinforced by carbon nanotubes (CNTs) and graphene-a review. Composites Part B:Engineering, 2015, 77: 402-420.
[24] GEIM A K.Graphene: status and prospects.Science, 2009, 324(19): 1530-1536.
[25] STOLLER M D, PARK S, ZHU Y, et al. Graphene-based ultracapacitors. Nano Letters, 2008, 8(10): 3498-3402.
[26] KUILLA T, BHADRA S, YAO D, et al. Recent advances in graphene based polymer composites. Progress in Polymer Science, 2010, 35(11): 1350-1375.
[27] KOTSYUBYNSKY V O, BOYCHUK V M, BUDZULIAK I M, et al. Structural properties of graphene oxide materials synthesized accordingly to Hummers, Tour and modified methods: XRD and Raman study. Physics and Chemistry of Solid State, 2021, 22(1): 31-38.
[28] MASTSUBARA C, KAWAMOTO N, TAKAMURA K.Oxo [5,10,15,20-tetra(4-pyridyl)porp hyrinatoltitanium (IV): an ultra- high sensitivity spectrophotometric reagent for hydrogen peroxide.Analyst, 1992, 117: 1781-1784.
[29] EISENBERG G.Colorimetric determination of hydrogen peroxide.Industrial & Engineering Chemistry, 1943, 15(5): 327-328.
[30] O'KANE S A, CLÉRAC R, ZHAO H, et al. New crystalline polymers of Ag(TCNQ) and Ag(TCNQF₄): structures and magnetic properties. Journal of Solid State Chemistry, 2000, 152(1): 159-173.
[31] ZHANG Q, ZHANG X, WANG J, et al. Graphene-supported single-atom catalysts and applications in electrocatalysis. Nanotechnology, 2021, 32(3): 1-24.
[32] MOHAN V B, LAU K T, HUI D, et al. Graphene-based materials and their composites: a review on production, applications and product limitations. Composites Part B: Engineering, 2018, 142: 200-220.
[33] HAN L, SUN Y, LI S, et al. In-plane carbon lattice-defect regulating electrochemical oxygen reduction to hydrogen peroxide production over nitrogen-doped graphene. ACS Catalysis, 2019, 9(2): 1283-1288.
[34] MALARD L M, PIMENTA M A, DRESSELHAUS G, et al. Raman spectroscopy in graphene. Physics Reports, 2009, 473(5/6): 51-87.
[35] JIRKOVSKY J S, PANAS I, AHLBERG E, et al. Single atom hot-spots at Au-Pd nanoalloys for electrocatalytic H₂O₂ production. Journal of the American Chemical Society, 2011, 133(48): 19432-19441.