AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
PDF (1.4 MB)
Submit Manuscript AI Chat Paper
Show Outline
Show full outline
Hide outline
Show full outline
Hide outline
Research Article | Open Access

Honeycomb-like MXene/NiFePx–NC with "continuous" single-crystal enabling high activity and robust durability in electrocatalytic oxygen evolution reactions

Xiaojun Zenga,c,( )Yifei Yea,Yongqing Wanga( )Ronghai YubMartin MoskovitscGalen D. Stuckyc( )
Advanced Ceramic Materials Research Institute, School of Materials Science and Engineering, Jingdezhen Ceramic University, Jingdezhen 333403, China
School of Materials Science and Engineering, Beihang University, Beijing 100191, China
Department of Chemistry and Biochemistry, University of California Santa Barbara, CA 93106, USA

† Xiaojun Zeng and Yifei Ye contributed equally to this work.

Show Author Information

Graphical Abstract


The development of low-cost, stable, and robust non-noble metal catalysts for water oxidation is a pivotal challenge for sustainable hydrogen production through electrocatalytic water splitting. Currently, such catalysts suffer from high overpotential and sluggish kinetics in oxygen evolution reactions (OERs). Herein, we report a "continuous" single-crystal honeycomb-like MXene/NiFePx–N-doped carbon (NC) heterostructure, in which ultrasmall NiFePx nanoparticles (NPs) encapsulated in the NC are tightly anchored on a layered MXene. Interestingly, this MXene/NiFePx–NC delivers outstanding OER catalytic performance, which stems from "continuous" single-crystal characteristics, abundant active sites derived from the ultrasmall NiFePx NPs, and the stable honeycomb-like heterostructure with an open structure. The experimental results are rationalized theoretically (by density functional theory (DFT) calculations), which suggests that it is the unique MXene/NiFePx–NC heterostructure that promotes the sluggish OER, thereby enabling superior durability and excellent activity with an ultralow overpotential of 240 mV at a current density of 10 mA·cm−2.

Electronic Supplementary Material

Download File(s)
JAC0704_ESM.pdf (3.8 MB)


Zhang L, Hu ZH, Huang JT, et al. Experimental and DFT studies of flower-like Ni-doped Mo2C on carbon fiber paper: A highly efficient and robust HER electrocatalyst modulated by Ni(NO3)2 concentration. J Adv Ceram 2022, 11: 1294–1306.
Chi JQ, Zeng XJ, Shang X, et al. Embedding RhPx in N,P co-doped carbon nanoshells through synergetic phosphorization and pyrolysis for efficient hydrogen evolution. Adv Funct Mater 2019, 29: 1901790.
Jiang WJ, Tang T, Zhang Y, et al. Synergistic modulation of non-precious-metal electrocatalysts for advanced water splitting. Acc Chem Res 2020, 53: 1111–1123.
Chen XZ, Ong WJ, Kong ZZ, et al. Probing the active sites of site-specific nitrogen doping in metal-free graphdiyne for electrochemical oxygen reduction reactions. Sci Bull 2020, 65: 45–54.
Kougias I, Taylor N, Kakoulaki G, et al. The role of photovoltaics for the European Green Deal and the recovery plan. Renew Sust Energ Rev 2021, 144: 111017.
McCrory CCL, Jung S, Ferrer IM, et al. Benchmarking hydrogen evolving reaction and oxygen evolving reaction electrocatalysts for solar water splitting devices. J Am Chem Soc 2015, 137: 4347–4357.
Yu ZJ, Mao KW, Feng Y. Single-source-precursor synthesis of porous W-containing SiC-based nanocomposites as hydrogen evolution reaction electrocatalysts. J Adv Ceram 2021, 10: 1338–1349.
Luo X, Ji PX, Wang PY, et al. Interface engineering of hierarchical branched Mo-doped Ni3S2/NixPy hollow heterostructure nanorods for efficient overall water splitting. Adv Energy Mater 2020, 10: 1903891.
Shen RC, Zhang LP, Chen XZ, et al. Integrating 2D/2D CdS/α-Fe2O3 ultrathin bilayer Z-scheme heterojunction with metallic β-NiS nanosheet-based ohmic-junction for efficient photocatalytic H2 evolution. Appl Catal B Environ 2020, 266: 118619.
Zeng X, Bai Y, Choi SM, et al. Mesoporous TiO2 nanospheres loaded with highly dispersed Pd nanoparticles for pH-universal hydrogen evolution reaction. Mater Today Nano 2019, 6: 100038.
Zhao EL, Du K, Yin P, et al. Advancing photoelectrochemical energy conversion through atomic design of catalysts. Adv Sci 2022, 9: 2104363.
Shan JQ, Zheng Y, Shi BY, et al. Regulating electrocatalysts via surface and interface engineering for acidic water electrooxidation. ACS Energy Lett 2019, 4: 2719–2730.
Zhao L, Zhang Y, Zhao ZL, et al. Steering elementary steps towards efficient alkaline hydrogen evolution via size-dependent Ni/NiO nanoscale heterosurfaces. Nat Sci Rev 2020, 7: 27–36.
Lv XD, Li XT, Yang C, et al. Large-size, porous, ultrathin NiCoP nanosheets for efficient electro/photocatalytic water splitting. Adv Funct Mater 2020, 30: 1910830.
Liang HF, Gandi AN, Anjum DH, et al. Plasma-assisted synthesis of NiCoP for efficient overall water splitting. Nano Lett 2016, 16: 7718–7725.
Lin Y, Sun KA, Liu SJ, et al. Construction of CoP/NiCoP nanotadpoles heterojunction interface for wide pH hydrogen evolution electrocatalysis and supercapacitor. Adv Energy Mater 2019, 9: 1901213.
Zeng XJ, Jang MJ, Choi SM, et al. Single-crystalline CoFe nanoparticles encapsulated in N-doped carbon nanotubes as a bifunctional catalyst for water splitting. Mater Chem Front 2020, 4: 2307–2313.
Nong SY, Dong WJ, Yin JW, et al. Well-dispersed ruthenium in mesoporous crystal TiO2 as an advanced electrocatalyst for hydrogen evolution reaction. J Am Chem Soc 2018, 140: 5719–5727.
Tung CW, Hsu YY, Shen YP, et al. Reversible adapting layer produces robust single-crystal electrocatalyst for oxygen evolution. Nat Commun 2015, 6: 8106.
Kuang Y, Zhang Y, Cai Z, et al. Single-crystalline dendritic bimetallic and multimetallic nanocubes. Chem Sci 2015, 6: 7122–7129.
Lv H, Qin HY, Sun MZ, et al. Mesoporosity-enabled selectivity of mesoporous palladium-based nanocrystals catalysts in semihydrogenation of alkynes. Angew Chem Int Ed Engl 2022, 61: e202114539.
Zeng XJ, Shui JL, Liu XF, et al. Single-atom to single-atom grafting of Pt1 onto Fe–N4 center: Pt1@Fe–N–C multifunctional electrocatalyst with significantly enhanced properties. Adv Energy Mater 2018, 8: 1701345.
Wang FH, Dong BB, Wang JW, et al. Self-supported porous heterostructure WC/WO3−x ceramic electrode for hydrogen evolution reaction in acidic and alkaline media. J Adv Ceram 2022, 11: 1208–1221.
Chang H, Li XZ, Shi LN, et al. Towards high-performance electrocatalysts and photocatalysts: Design and construction of MXenes-based nanocomposites for water splitting. Chem Eng J 2021, 421: 129944.
Guo DZ, Li X, Jiao YQ, et al. A dual-active Co–CoO heterojunction coupled with Ti3C2-MXene for highly-performance overall water splitting. Nano Res 2022, 15: 238–247.
Zeng XJ, Duan DR, Zhang XF, et al. Doping and interface engineering in a sandwich Ti3C2Tx/MoS2−xPx heterostructure for efficient hydrogen evolution. J Mater Chem C 2022, 10: 4140–4147.
Zeng XJ, Zhao Y, Hu XD, et al. Rational component and structure design of noble-metal composites for optical and catalytic applications. Small Struct 2021, 2: 2000138.
Lv ZP, Ma WS, Wang M, et al. Co-constructing interfaces of multiheterostructure on MXene (Ti3C2Tx)-modified 3D self-supporting electrode for ultraefficient electrocatalytic HER in alkaline media. Adv Funct Mater 2021, 31: 2102576.
Zheng ZX, Wu W, Yang T, et al. In situ reduced MXene/ AuNPs composite toward enhanced charging/discharging and specific capacitance. J Adv Ceram 2021, 10: 1061–1071.
Yang LM, Yang T, Chen YF, et al. FeNi LDH/V2CTx/NF as self-supported bifunctional electrocatalyst for highly effective overall water splitting. Nanomaterials-Basel 2022, 12: 2640.
Xue Y, Zheng YP, Wang EH, et al. Ti3C2Tx (MXene)/Pt nanoparticle electrode for the accurate detection of DA coexisting with AA and UA. Dalton Trans 2022, 51: 4549–4559.
Zheng ZX, Guo CY, Wang EH, et al. The oxidation and thermal stability of two-dimensional transition metal carbides and/or carbonitrides (MXenes) and the improvement based on their surface state. Inorg Chem Front 2021, 8: 2164–2182.
Chen XX, Li MS, Hou J, et al. Molten salt method synthesis of multivalent cobalt and oxygen vacancy modified nitrogen-doped MXene as highly efficient hydrogen and oxygen Evolution reaction electrocatalysts. J Colloid Interf Sci 2022, 615: 831–839.
Wang ZW, Wu YC, Zhu YH, et al. Exploring the mechanism of electrocatalytic water oxidation on CoO decorated Ti3C2Tx nanoplatelets. Electrochimica Acta 2022, 409: 139969.
Peng C, Kuai ZY, Zeng TQ, et al. WO3 Nanorods/MXene composite as high performance electrode for supercapacitors. J Alloys Compd 2019, 810: 151928.
Sun SB, Wang MW, Chang XT, et al. W18O49/Ti3C2Tx MXene nanocomposites for highly sensitive acetone gas sensor with low detection limit. Sensor Actuat B-Chem 2020, 304: 127274.
Deng RX, Chen BB, Li HG, et al. MXene/Co3O4 composite material: Stable synthesis and its enhanced broadband microwave absorption. Appl Surf Sci 2019, 488: 921–930.
Guo JQ, Zhan ZX, Lei T, et al. Self-supported FeNiP nanosheet arrays as a robust bifunctional electrocatalyst for water splitting. ACS Appl Energy Mater 2022, 5: 5855–5866.
Cao Y, Deng QH, Liu ZD, et al. Enhanced thermal properties of poly(vinylidene fluoride) composites with ultrathin nanosheets of MXene. RSC Adv 2017, 7: 20494–20501.
Zhou BJ, Liu YY, Wu XL, et al. Wood-derived integrated air electrode with Co–N sites for rechargeable zinc-air batteries. Nano Res 2022, 15: 1415–1423.
Bao WZ, Tang X, Guo X, et al. Porous cryo-dried MXene for efficient capacitive deionization. Joule 2018, 2: 778–787.
Yan P, Liu Q, Zhang H, et al. Deeply reconstructed hierarchical and defective NiOOH/FeOOH nanoboxes with accelerated kinetics for the oxygen evolution reaction. J Mater Chem A 2021, 9: 15586–15594.
Hei JC, Xu GC, Wei B, et al. NiFeP nanosheets on N-doped carbon sponge as a hierarchically structured bifunctional electrocatalyst for efficient overall water splitting. Appl Surf Sci 2021, 549: 149297.
Zhao DY, Zhao RZ, Dong SH, et al. Alkali-induced 3D crinkled porous Ti3C2 MXene architectures coupled with NiCoP bimetallic phosphide nanoparticles as anodes for high-performance sodium-ion batteries. Energy Environ Sci 2019, 12: 2422–2432.
Wan L, He CY, Chen DQ, et al. In situ grown NiFeP@NiCo2S4 nanosheet arrays on carbon cloth for asymmetric supercapacitors. Chem Eng J 2020, 399: 125778.
Diao FY, Huang W, Ctistis G, et al. Bifunctional and self-supported NiFeP-layer-coated NiP rods for electrochemical water splitting in alkaline solution. ACS Appl Mater Interfaces 2021, 13: 23702–23713.
Li Y, Wei B, Yu ZP, et al. Bifunctional porous cobalt phosphide foam for high-current-density alkaline water electrolysis with 4000-h long stability. ACS Sustainable Chem Eng 2020, 8: 10193–10200.
Yang WZ, Huang BY, Li LB, et al. Covalently sandwiching MXene by conjugated microporous polymers with excellent stability for supercapacitors. Small Methods 2020, 4: 2000434.
Pazniak A, Bazhin P, Shplis N, et al. Ti3C2Tx MXene characterization produced from SHS-ground Ti3AlC2. Mater Des 2019, 183: 108143.
Zeng XJ, Zhao C, Yin YC, et al. Construction of NiCo2O4 nanosheets-covered Ti3C2Tx MXene heterostructure for remarkable electromagnetic microwave absorption. Carbon 2022, 193: 26–34.
Zang R, Li PX, Guo X, et al. Yolk–shell N-doped carbon coated FeS2 nanocages as a highperformance anode for sodium-ion batteries. J Mater Chem A 2019, 7: 14051–14059.
Zai SF, Gao XY, Yang CC, et al. Ce-modified Ni(OH)2 nanoflowers supported on NiSe2 octahedra nanoparticles as high-efficient oxygen evolution electrocatalyst. Adv Energy Mater 2021, 11: 2101266.
Sun HM, Yan ZH, Liu FM, et al. Self-supported transition-metal-based electrocatalysts for hydrogen and oxygen evolution. Adv Mater 2020, 32: 1806326.
Wang JZ, Chen C, Cai N, et al. High topological tri-metal phosphide of CoP@FeNiP toward enhanced activities in oxygen evolution reaction. Nanoscale 2021, 13: 1354–1363.
Du YM, Han Y, Huai XD, et al. N-doped carbon coated FeNiP nanoparticles based hollow microboxes for overall water splitting in alkaline medium. Int J Hydrogen Energy 2018, 43: 22226–22234.
Gong YX, Xu LH, Li JJ, et al. Confinement of transition metal phosphides in N, P-doped electrospun carbon fibers for enhanced electrocatalytic hydrogen evolution. J Alloys Compd 2021, 875: 159934.
Bu FX, Chen WS, Aly Aboud MF, et al. Microwave-assisted ultrafast synthesis of adjustable bimetal phosphide/ graphene heterostructures from MOFs for efficient electrochemical water splitting. J Mater Chem A 2019, 7: 14526–14535.
Qian MM, Cui SS, Jiang DC, et al. Highly efficient and stable water-oxidation electrocatalysis with a very low overpotential using FeNiP substitutional-solid-solution nanoplate arrays. Adv Mater 2017, 29: 1704075.
Cai Z, Bi YM, Hu EY, et al. Single-crystalline ultrathin Co3O4 nanosheets with massive vacancy defects for enhanced electrocatalysis. Adv Energy Mater 2018, 8: 1701694.
Wang YS, Li YY, Qiu ZP, et al. Fe3O4@Ti3C2 MXene hybrids with ultrahigh volumetric capacity as an anode material for lithium-ion batteries. J Mater Chem A 2018, 6: 11189–11197.
Dai BZ, Zhao B, Xie X, et al. Novel two-dimensional Ti3C2Tx MXenes/nano-carbon sphere hybrids for high-performance microwave absorption. J Mater Chem C 2018, 6: 5690–5697.
Zhao GL, Lv HP, Zhou Y, et al. Self-assembled sandwich-like MXene-derived nanocomposites for enhanced electromagnetic wave absorption. ACS Appl Mater Interfaces 2018, 10: 42925–42932.
Zeng XJ, Zhang QQ, Shen ZY, et al. Doping and vacancy engineering in a sandwich-like g-C3N4/NiCo2O4 heterostructure for robust oxygen evolution. ChemNanoMat 2022, 8: e202200191.
Chen S, Huang H, Jiang P, et al. Mn-doped RuO2 nanocrystals as highly active electrocatalysts for enhanced oxygen evolution in acidic media. ACS Catal 2020, 10: 1152–1160.
Journal of Advanced Ceramics
Pages 553-564
Cite this article:
Zeng X, Ye Y, Wang Y, et al. Honeycomb-like MXene/NiFePx–NC with "continuous" single-crystal enabling high activity and robust durability in electrocatalytic oxygen evolution reactions. Journal of Advanced Ceramics, 2023, 12(3): 553-564.








Web of Science






Received: 20 September 2022
Accepted: 05 December 2022
Published: 16 February 2023
© The Author(s) 2022.

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit