Defective graphene synergizes with NiOx nanosheets to facilitate dual-defect-assisted two-electron oxygen reduction

Run Huang , Helong Wu , Qingchao Fang , Ying Chen , Panjie Guo , Xuan Liu , Mengting Huang , Jinyan Zhang , Aijun Du , Lei Wang , Xin Wang

Chemical Synthesis ›› 2026, Vol. 6 ›› Issue (3) -46.

PDF
Chemical Synthesis ›› 2026, Vol. 6 ›› Issue (3) -46. DOI: 10.20517/cs.2024.172
Research Article
Defective graphene synergizes with NiOx nanosheets to facilitate dual-defect-assisted two-electron oxygen reduction
Author information +
History +
PDF

Abstract

One of the biggest challenges in the electrochemical synthesis of H2O2 is the development of high-performance and economical catalysts. In this work, a two-dimensional composite material consisting of NiOx nanosheets and defective graphene (DG) (NiOx@DG) was prepared and showed excellent electrocatalytic performance toward electrosynthesis of H2O2 from oxygen reduction reaction. Particularly, the NiOx@DG catalysts present superior activity indicators to physical mixing counterparts (NiOx-DG), encompassing a high onset potential of 0.78 V, high efficiency and 2e- selectivity over a wide potential range between 0.20-0.60 V (maximal value of 95%). The high activity of NiOx@DG can be attributed to the dual-defects (oxygen vacancies on NiOx and topological defects on DG)-induced strong electronic metal–support interaction. Such multi-defects collaborative enhancement strategy may provide a promising avenue for the preparation of high-performance catalysts toward application in different reactions.

Keywords

NiOx@DG / oxygen reduction reactions / hydrogen peroxide / electrocatalysis

Cite this article

Download citation ▾
Run Huang, Helong Wu, Qingchao Fang, Ying Chen, Panjie Guo, Xuan Liu, Mengting Huang, Jinyan Zhang, Aijun Du, Lei Wang, Xin Wang. Defective graphene synergizes with NiOx nanosheets to facilitate dual-defect-assisted two-electron oxygen reduction. Chemical Synthesis, 2026, 6(3): -46 DOI:10.20517/cs.2024.172

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

Jiang Y,Chen C.Selective electrochemical H2O2 production through two-electron oxygen electrochemistry.Adv Energy Mater2018;8:1801909

[2]

Sun Y,Strasser P.A comparative perspective of electrochemical and photochemical approaches for catalytic H2O2 production.Chem Soc Rev2020;49:6605-31

[3]

Wu Z,Zou J,Zhang C.Amorphous nickel oxides supported on carbon nanosheets as high-performance catalysts for electrochemical synthesis of hydrogen peroxide.ACS Catal2022;12:5911-20

[4]

Tian Q,Wang W.Utilizing carbonaceous catalysts for H2O2 electrosynthesis via the two-electron oxygen reduction reaction.Energy Lab2025;3:240019

[5]

Liu W,Zhang J.Tuning the atomic configuration of Co-N-C electrocatalyst enables highly-selective H2O2 production in acidic media.Appl Catal B Environ2022;310:121312

[6]

Jirkovský JS,Ahlberg E,Romani S.Single atom hot-spots at Au-Pd nanoalloys for electrocatalytic H2O2 production.J Am Chem Soc2011;133:19432-41

[7]

Siahrostami S,Karamad M.Enabling direct H2O2 production through rational electrocatalyst design.Nat Mater2013;12:1137-43

[8]

Ko Y,Yang B.A catalyst design for selective electrochemical reactions: direct production of hydrogen peroxide in advanced electrochemical oxidation.J Mater Chem A2020;8:9859-70

[9]

Xie J,Yang X.Phosphorous and selenium tuning Co-based non-precious catalysts for electrosynthesis of H2O2 in acidic media.Chin Chem Lett2024;35:108472

[10]

Jung E,Lee BH.Atomic-level tuning of Co-N-C catalyst for high-performance electrochemical H2O2 production.Nat Mater2020;19:436-42

[11]

Yan L,Wang Y.Exsolved Co3O4 with tunable oxygen vacancies for electrocatalytic H2O2 production.Mater Today Energy2022;24:100931

[12]

Sun Y,Ju W.Efficient electrochemical hydrogen peroxide production from molecular oxygen on nitrogen-doped mesoporous carbon catalysts.ACS Catal2018;8:2844-56

[13]

Liu Y,Fan X,Chen S.High-yield electrosynthesis of hydrogen peroxide from oxygen reduction by hierarchically porous carbon.Angew Chem2015;127:6941-5

[14]

Wang M,Feng Y,Shao Q.Partially pyrolyzed binary metal-organic framework nanosheets for efficient electrochemical hydrogen peroxide synthesis.Angew Chem Int Ed Engl2020;59:14373-7

[15]

Cai P,Chen J.Oxygen-containing amorphous cobalt sulfide porous nanocubes as high-activity electrocatalysts for the oxygen evolution reaction in an alkaline/neutral medium.Angew Chem Int Ed Engl2017;56:4858-61

[16]

Indra A,Zaharieva I.Active mixed-valent MnOx water oxidation catalysts through partial oxidation (corrosion) of nanostructured MnO particles.Angew Chem Int Ed Engl2013;52:13206-10

[17]

Yin S,Sheng Y.A highly efficient oxygen evolution catalyst consisting of interconnected nickel-iron-layered double hydroxide and carbon nanodomains.Adv Mater2018;30:1705106

[18]

Zhang C,Daly K,Trudel S.Water oxidation catalysis: tuning the electrocatalytic properties of amorphous lanthanum cobaltite through calcium doping.ACS Catal2017;7:6385-91

[19]

Smith RD,Fagan RD.Photochemical route for accessing amorphous metal oxide materials for water oxidation catalysis.Science2013;340:60-3

[20]

Pan L,Li Y.Amorphous cobalt-cerium binary metal oxides as high performance electrocatalyst for oxygen evolution reaction.J Catal2020;384:14-21

[21]

Li X,Li D,Tao H.Amorphous alloys for electrocatalysis: the significant role of the amorphous alloy structure.Nano Res2023;16:4277-88

[22]

Xia Y,Xia C.Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates.Nat Commun2021;12:24329 PMCID:PMC8270976

[23]

Jiao Y,Jaroniec M.Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance.J Am Chem Soc2014;136:4394-403 PMCID:PMC3986026

[24]

Chen G,Li Q.A direct H2O2 production based on hollow porous carbon sphere-sulfur nanocrystal composites by confinement effect as oxygen reduction electrocatalysts.Nano Res2019;12:2614-22

[25]

Zhang J,He F.Defect and doping Co-engineered non-metal nanocarbon ORR electrocatalyst.Nanomicro Lett2021;13:65 PMCID:PMC8187682

[26]

Melchionna M,Prato M.The rise of hydrogen peroxide as the main product by metal-free catalysis in oxygen reductions.Adv Mater2019;31:1802920

[27]

Chen S,Siahrostami S.Defective carbon-based materials for the electrochemical synthesis of hydrogen peroxide.ACS Sustainable Chem Eng2018;6:311-7

[28]

Zhang L,Niu J.Role of lattice defects in catalytic activities of graphene clusters for fuel cells.Phys Chem Chem Phys2015;17:16733-43

[29]

Zhu J,Mei W.Effects of intrinsic pentagon defects on electrochemical reactivity of carbon nanomaterials.Angew Chem Int Ed2019;58:3859-64

[30]

Wang W,Chang G.Intrinsic carbon-defect-driven electrocatalytic reduction of carbon dioxide.Adv Mater2019;31:e1808276

[31]

Huang J,Chen J,Peng X.The enhancement of selectivity and activity for two-electron oxygen reduction reaction by tuned oxygen defects on amorphous hydroxide catalysts.CCS Chem2022;4:566-83

[32]

Shen S,Guo P.Effect of Cr doping on the photoelectrochemical performance of hematite nanorod photoanodes.Nano Energy2012;1:732-41

[33]

Paulus UA,Gasteiger HA.Oxygen reduction on a high-surface area Pt:Vulcan carbon catalyst: a thin-film rotating ring-disk electrode study.J Electroanal Chem2001;495:134-45

[34]

FLOOD H.The acidic and basic properties of oxides.Acta Chem Scand1947;1:592-604

[35]

Deming CP,Gadiraju V,Khan M.Graphene quantum dots-supported palladium nanoparticles for efficient electrocatalytic reduction of oxygen in alkaline media.ACS Sustainable Chem Eng2015;3:3315-23

[36]

Liu Q,He Z,Chen Y.A facile top-down approach for constructing perovskite oxide nanostructure with abundant oxygen defects as highly efficient water oxidation electrocatalyst.Int J Hydrogen Energy2020;45:22808-16

[37]

Kim C,Kwak SK,Kim G.Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide.Nat Commun2023;14:41397 PMCID:PMC10509222

[38]

Wei Z,Zhang C,Lu X.Reversed charge transfer and enhanced hydrogen spillover in platinum nanoclusters anchored on titanium oxide with rich oxygen vacancies boost hydrogen evolution reaction.Angew Chem Int Ed2021;60:16622-7

[39]

Huang H,Liu D.Tailoring oxygen reduction reaction kinetics on perovskite oxides via oxygen vacancies for low-temperature and knittable Zinc-air batteries.Adv Mater2023;35:e2303109

[40]

Shao Z,Sun Y.Phase-reconfiguration-induced NiS/NiFe2O4 composite for performance-enhanced Zinc-air batteries.Adv Mater2022;34:e2110172

[41]

Lepre E,Nowakowski M.Ni-based electrocatalysts for unconventional CO2 reduction reaction to formic acid.Nano Energy2022;97:107191

[42]

Choi CH,Kwon HC.Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst.Nat Commun2016;7:10922 PMCID:PMC4786782

[43]

Kim HW,Kornienko N.Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts.Nat Catal2018;1:282-90

[44]

Sa YJ,Joo SH.Active edge-site-rich carbon nanocatalysts with enhanced electron transfer for efficient electrochemical hydrogen peroxide production.Angew Chem Int Ed2019;58:1100-5

[45]

Lei X,Zheng Y.High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis.Nat Sustain2023;6:816-26

[46]

Tian Q,Du H.Mesoporous carbon spheres with programmable interiors as efficient nanoreactors for H2O2 electrosynthesis.Nat Commun2024;15:983 PMCID:PMC10834542

[47]

Zhi Q,Yang X.Dithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable H2O2 electroproduction.Nat Commun2024;15:678 PMCID:PMC10805717

[48]

Tian Y,Wu Z.Edge-hosted atomic Co-N4 sites on hierarchical porous carbon for highly selective two-electron oxygen reduction reaction.Angew Chem Int Ed Engl2022;61:e202213296 PMCID:PMC10098864

PDF

0

Accesses

0

Citation

Detail

Sections
Recommended

/