纳米金刚石改性及其在电催化氧还原反应中的应用

doi:10.15541/jim20250135

无机材料学报 ›› 2026, Vol. 41 ›› Issue (3): 273-288.DOI: 10.15541/jim20250135 CSTR: 32189.14.jim20250135

• 综述 • 下一篇

纳米金刚石改性及其在电催化氧还原反应中的应用

韦连金(), 齐志杰, 汪信, 朱俊武, 付永胜()

南京理工大学软化学与功能材料教育部重点实验室, 南京 210094

收稿日期:2025-03-31 修回日期:2025-07-10 出版日期:2025-08-26 网络出版日期:2025-08-26
通讯作者: 付永胜, 教授. E-mail: fuyongsheng@njust.edu.cn
作者简介:韦连金(2003-), 男, 博士研究生. E-mail: 3259728845@qq.com
基金资助:
国家自然科学基金(52173255)

Modification of Nanodiamond and Its Application in Electrocatalytic Oxygen Reduction Reaction

WEI Lianjin(), QI Zhijie, WANG Xin, ZHU Junwu, FU Yongsheng()

Key Laboratory for Soft Chemistry and Functional Materials, Ministry of Education, Nanjing University of Science and Technology, Nanjing 210094, China

Received:2025-03-31 Revised:2025-07-10 Published:2025-08-26 Online:2025-08-26
Contact: FU Yongsheng, professor. E-mail: fuyongsheng@njust.edu.cn
About author:WEI Lianjin (2003-), male, PhD candidate. E-mail: 3259728845@qq.com
Supported by:
National Natural Science Foundation of China(52173255)

摘要/Abstract

摘要：

氧还原反应(Oxygen reduction reaction, ORR)作为燃料电池和金属空气电池等清洁能源装置的关键阴极反应, 反应动力学缓慢, 使其实际应用受到了严重制约。虽然铂(Pt)基催化剂具有出色的ORR活性, 但其价格昂贵、储量稀缺、稳定性和耐受性差, 极大地阻碍了商业化进程。因此, 开发高效、低成本的新型ORR催化剂成为当前研究的重点。纳米金刚石(Nanodiamond, ND)的成本低、官能团修饰可控、表面能高(>1000 mJ·m^-2)且具有独特π和σ电子结构, 作为新兴碳基材料在ORR催化中极具潜力。本文综述了ND催化剂的最新研究进展, 首先介绍了爆轰法、化学气相沉积法、脉冲激光烧蚀法、高温高压法等制备方法, 随后总结了杂原子掺杂、表面功能化、材料复合及形貌调控等改性策略, 并分析了活性中心形成机制与反应路径调控规律, 涵盖不同改性策略对催化性能的影响及相关性能数据对比。最后探讨了当前ND催化剂在催化机理、合成工艺、表征技术及设计方法等方面面临的挑战, 并展望了未来发展方向, 为研发新型碳基ORR催化剂提供了参考。

关键词: 纳米金刚石, 化学改性, 电催化, 氧还原反应, 综述

Abstract:

Oxygen reduction reaction (ORR) is an important cathodic reaction, but its slow reaction kinetics seriously hinders the application of clean energy devices such as fuel cells and metal-air batteries. Although platinum (Pt)-based catalysts possess excellent ORR activity, their high cost, scarce reserves, poor stability and tolerance make it difficult to commercialize current clean energy technologies. To address the above problems, it is urgent to develop new types of efficient and low-cost ORR catalysts. As an emerging carbon-based material, nanodiamond (ND) exhibits broad application prospects in ORR catalysis due to its advantages such as low cost, controllable functional group modification, high surface energy (>1000 mJ·m^-2), and unique π and σ bond configurations. This paper reviews the latest research progress of ND catalysts. Firstly, preparation methods such as detonation, chemical vapor deposition, pulsed laser ablation, and high-pressure high-temperature are introduced. Subsequently, modification strategies including heteroatom doping, surface functionalization, material composite, and morphology regulation are summarized, and their formation mechanism of active centers and regulation rules of reaction paths are analyzed, covering influence of different modification strategies on catalytic performance and comparison of relevant performance data. Finally, the challenges faced by current ND catalysts in catalytic mechanism, synthesis process, characterization technology, and design methods are analyzed to suggest the future development directions for the research and development of new carbon-based ORR catalysts.

Key words: nanodiamond, chemical modification, electrocatalysis, oxygen reduction reaction, review

中图分类号:

O646

韦连金, 齐志杰, 汪信, 朱俊武, 付永胜. 纳米金刚石改性及其在电催化氧还原反应中的应用[J]. 无机材料学报, 2026, 41(3): 273-288.

WEI Lianjin, QI Zhijie, WANG Xin, ZHU Junwu, FU Yongsheng. Modification of Nanodiamond and Its Application in Electrocatalytic Oxygen Reduction Reaction[J]. Journal of Inorganic Materials, 2026, 41(3): 273-288.

图/表 13

图1 应用于ORR的ND改性策略

Fig. 1 Modification of ND for ORR

图2 ND的结构示意图模型[14]

Fig. 2 Schematic model of the ND structure[14] (a) Schematic model illustrating structure of detonation ND; (b) Closer view of surface region of ND covered with surface functional groups and sp2 carbon; (c) Illustration of sp3 carbon framework in the core

图3 不同制备方法得到的ND的拉曼谱图[34,37,43,49]

Fig. 3 Raman spectra of ND prepared by different methods[34,37,43,49] (a) DND[34]; (b) CVD under different methane concentrations[37]; (c) PLA[43]; (d) HPHT at different temperatures[49]

表1 酸性和碱性电解液中的阴极ORR路径[55] (E0: 标准电位)

Table 1 Cathodic ORR path in acid and alkaline electrolytes[55] (E0: standard potential)

ORR pathway	2e^-	4e^-
Acid electrolyte	O₂+2H⁺+2e^-→H₂O₂ (E⁰=0.67 V (vs. RHE)) O₂+→O₂ O₂+H⁺+e^-→OOH OOH+H⁺+e^-→H₂O₂+	O₂+4H⁺+4e^-→2H₂O (E⁰=1.23 V (vs. RHE)) O₂+→O₂
		O₂+H⁺+e^-→OOH
		OOH+H+e^-→O+H₂O
		O+H⁺+e^-→OH
		OH+H⁺+e^-→H₂O+
Alkaline electrolyte	O₂+2H₂O+2e^-→HO₂^-+OH^- (E⁰=0.065 V (vs. RHE))	O₂+2H₂O+4e^-→4OH^- (E⁰=0.40 V (vs. RHE)) O₂+→O₂ O₂+H₂O+e^-→OOH+OH^- OOH+e^-→O+OH^- O+H₂O+e^-→OH^-+OH^- OH^-+e^-→OH^-+
Alkaline electrolyte	HO₂^-+H₂O+2e^-→3OH^- (E⁰=0.867 V (vs. RHE))

图4 通过2e-或4e-转移途径的ORR机制[56]

Fig. 4 Mechanism of ORR via 2e- or 4e- transfer pathway[56]

图5 基于杂原子掺杂的各种研究[64,68,70-71]

Fig. 5 Various studies based on heteroatom doping[64,68,70-71] (a) Schematic diagram of preparation process of BND and Pt1/BND[64]; (b) Structure of OOH adsorption, charge density (up) and PDOS (down) for OOH adsorption on BND surface[64]; (c) Free-energy profile of 2e− ORR at 0.68 V (vs. RHE) on BND and Pt1/BND[64]; (d, e) Adsorption energies of (d) ΔG*OOH and (e) ΔG*H2O2 on the surface of raw D, BND, and Pt1/BND[64]; (f) LSV curves of ND, NO, NNO-xh, and Pt/C samples[68]; (g) RDE voltammograms recorded with OLC-1, B-OLC-1-5, B-OLC-1-10, B-OLC-1-20, and Pt/C in O2-saturated 0.1 mol·L-1 KOH at 900 r·min-1 with a scan rate of 5 mV·s−1[70]; (h) LSV curves of OLC with different phosphate loading[71]

图6 ND随温度升高表面结构的变化[74]

Fig. 6 Change of surface structure of ND with the increase of temperature[74]

图7 ND的表面处理[77,79]

Fig. 7 Surface treatment of ND[77,79] (a) Relationship between ORR activity and degree of defect based on sp2-C bandwidth in C1s XPS spectra[77]; (b) ORR voltammograms of samples prepared at different temperatures[77]; (c) Changes in ORR activity at-10 μA·cm-2 for heat-treated NDs at different preparation temperatures[77]; (d, e) In situ attenuated total reflectance infrared (ATR-IR) spectra under different potential conditions in O2-saturated environment of (d) ND and (e) ND(PH)[79]; (f, g) Schematic diagrams of possible reaction pathways for carbonyl sites on ND (gray: C atom, red: O atom, white: H atom, *: active site)[79]; (h) Free energies of key intermediates occurring at two sites on pathway A and pathway B[79]

图8 POM@CDNPs复合材料的制备和性能[83]

Fig. 8 Preparation and property of POM@CDNPs composites[83] (a) Preparative schematic of POM@CDNPs composite; (b) LSV comparison of electrocatalysts recorded at 3000 r·min-1 with a scan rate of 5 mV·s-1; (c) Transfer electron numbers of CDNP and POM@CDNPs

图9 WS2/NiO/ND/C和MoS2/NiO/ND/C的制备与性能[84]

Fig. 9 Preparation and performance of WS2/NiO/ND/C and MoS2/NiO/ND/C[84] (a) Schematic illustration for preparation of MoS2/NiO/ND/C and WS2/NiO/ND/C nanocomposites; (b) Number of transferred electrons; (c) Chronoamperometric curve of WS2/NiO/ND/C in 0.1 mol·L-1 KOH for 54000 s

图10 基于形貌调控ND电催化剂的制备与性能[91-92]

Fig. 10 Preparation and performance of ND electrocatalyst based on morphology regulation[91-92] (a) SEM image of BND2[91]; (b) ORR polarization curves of different catalysts at a rotational speed of 1400 r·min-1[91]; (c) Polarization and power density curves for zinc-air batteries with BND2 and Pt/C catalysts[91]; (d) Evaluation of durability of BND2 and Pt/C catalysts at-0.2 V (0.1 mol·L-1 KOH in saturated O2)[91]; (e) Discharge curves of zinc-air batteries with BND2 and Pt/C catalysts at a current density of 30.0 mA·cm-2[91]; (f) SEM image of BDD catalyst deposited on a foamed nickel substrate[92]; (g) LSV curves, (h) electron transfer numbers and (i) methanol tolerance tests for different SSA samples and Pt/C (I to IV represent samples with increasing SSA)[92]

图11 N-CNWs/D材料的制备与性能[93]

Fig. 11 Preparation and performance of N-CNWs/D material[93] (a) Illustration of preparation of Ar-treated N-CNWs/D films; (b) SEM image of N-CNWs/D-9 films after Ar annealing treatment at 600 ℃; (c, d) HRTEM images of N-CNWs/D-9 (c) before and (d) after Ar annealing at 600 ℃; (e) Raman spectra of N-CNWs/D-9 films after Ar annealing at different temperatures; (f) LSV curves of N-CNWs/D-9 films treated with Ar at different temperatures; (g) Chronoamperometric curves of Ar-treated N-CNWs/D-9 films and Pt/C in 0.1 mol·L-1 KOH solution before and after addition of methanol

表2 部分ND催化剂性能汇总

Table 2 Summary of properties of some ND catalysts

Catalyst	E_onset/V (vs. RHE)	E_1/2/V (vs. RHE)	J_L/(mA·cm⁻²)	Transferred electrons, n	Ref.
BN-C/ND	0.75	0.69	−5.98	3.8	[65]
Co-N-C/ND	0.89	0.76	−4.31	3.8	[72]
ND/Fe₃C@Fe-N-C	0.89	0.80	−4.25	3.9	[73]
NNO-6h	0.81	0.71	−4.23	3.3	[68]
B-OLC-1-10	0.80	0.734	‒3.74	3.95	[70]
N-GND	0.89	0.82	‒4.63	3.8	[78]
NDGNSs	0.93	0.783	‒4.45	3.95	[82]
POM@CDNPs	0.85	0.773	−7.30	4.1	[83]
ND/N-G	0.97	0.773	‒4.61	3.65	[69]
WS₂/NiO/ND/C	0.76	0.63	−7.47	4.0	[84]
BND2	0.96	0.83	‒5.34	3.96	[91]
BDD	0.94	0.80	‒2.62	3.45	[92]
N-CNWs/D-9	0.84	0.72	−4.18	3.86	[93]
BND	0.73	-	-	2.19	[64]

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纳米金刚石改性及其在电催化氧还原反应中的应用

Modification of Nanodiamond and Its Application in Electrocatalytic Oxygen Reduction Reaction

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