氮掺杂碳载体负载钌纳米颗粒及其电解水析氢性能研究
Research on Ru Nanoparticles Loaded on N-Doping Carbon Support for Electrochemical Hydrogen Evolution Reaction
摘要: 金属–载体相互作用在调控金属纳米颗粒的电子结构及其稳定金属纳米颗粒方面发挥着关键作用。本研究以具有独特空腔结构的葫芦[6]脲(CB6)为前驱体，通过水热合成结合高温热解的策略，成功制备了氮掺杂碳负载钌纳米颗粒催化剂(Ru/CN)。系统研究了合成过程中前驱体不同处理工艺及不同煅烧温度对材料结构和电催化析氢性能的影响。电化学测试结果表明，所制备的Ru/CN催化剂在碱性电解液中表现出优异的析氢反应性能，达到10 mA cm–2电流密度时仅需12 mV的过电位，且在10 mA cm–2恒定电流密度下连续电解220小时后仍保持优异的催化稳定性，展现出显著的性能优势。这一发现为设计高效稳定的HER电催化剂提供了新的思路和实验依据。
Abstract: Metal-support interaction is vital of modulating electronic structure of metal nanoparticles as well as stabilizing these nanoparticles. In this study, nitrogen-doped carbon-loaded ruthenium nanoparticle catalysts (Ru/CN) were successfully prepared by hydrothermal synthesis combined with high-temperature pyrolysis strategy using cucurbit [6] uril (CB6), which has a unique cavity structure, as a precursor. The effects of different treatment processes of precursors and different calcination temperatures on the structure and electrocatalytic hydrogen reaction performance of the materials during the synthesis were systematically investigated. The electrochemical test results showed that the prepared Ru/CN catalyst exhibited excellent hydrogen reaction performance in alkaline electrolyte, requiring only 12 mV overpotential to reach 10 mA cm−2 current density, and maintained excellent catalytic stability after 220 h of continuous electrolysis at a constant current density of 10 mA cm−2, demonstrating significant performance advantages. This finding provides a new idea and experimental basis for the design of efficient and stable HER electrocatalysts.
文章引用：孟子琪, 冯家迅, 刘亚楠, 刘梦冉, 孙旭镯, 李波. 氮掺杂碳载体负载钌纳米颗粒及其电解水析氢性能研究[J]. 物理化学进展, 2025, 14(2): 264-273. https://doi.org/10.12677/japc.2025.142025

参考文献

[1] Tang, R., Yang, Y., Zhou, Y. and Yu, X. (2023) Rational Design of Heterostructured Ru Cluster‐Based Catalyst for pH Universal Hydrogen Evolution Reaction and High‐performance Zn‐H2O Battery. Advanced Functional Materials, 34, Article ID: 2301925. [Google Scholar] [CrossRef] 
[2] Jadhav, H.S., Bandal, H.A., Ramakrishna, S. and Kim, H. (2022) Critical Review, Recent Updates on Zeolitic Imidazolate Framework‐67 (ZIF‐67) and Its Derivatives for Electrochemical Water Splitting. Advanced Materials, 34, Article ID: 2107072. [Google Scholar] [CrossRef] [PubMed]
[3] Luo, Y., Zhang, Z., Chhowalla, M. and Liu, B. (2022) Recent Advances in Design of Electrocatalysts for High‐Current‐density Water Splitting. Advanced Materials, 34, Article ID: 2108133. [Google Scholar] [CrossRef] [PubMed]
[4] Faber, M.S. and Jin, S. (2014) Earth-Abundant Inorganic Electrocatalysts and Their Nanostructures for Energy Conversion Applications. Energy & Environmental Science, 7, 3519-3542. [Google Scholar] [CrossRef] 
[5] Li, Z., Li, X., Ma, H., Ye, C., Yu, H., Nie, L., et al. (2024) Anchoring Ru Clusters to Highly Defective N-Doped Carbon Nanotubes via a Thermal-Shock Strategy for Stable Industrial Hydrogen Evolution. Nano Research, 17, 5261-5269. [Google Scholar] [CrossRef] 
[6] Luo, W., Wang, Y. and Cheng, C. (2020) Ru-Based Electrocatalysts for Hydrogen Evolution Reaction: Recent Research Advances and Perspectives. Materials Today Physics, 15, Article ID: 100274. [Google Scholar] [CrossRef] 
[7] Higgins, S. (2010) Regarding Ruthenium. Nature Chemistry, 2, 1100. [Google Scholar] [CrossRef] [PubMed]
[8] Mahmood, J., Li, F., Jung, S., Okyay, M.S., Ahmad, I., Kim, S., et al. (2017) An Efficient and pH-Universal Ruthenium-Based Catalyst for the Hydrogen Evolution Reaction. Nature Nanotechnology, 12, 441-446. [Google Scholar] [CrossRef] [PubMed]
[9] Yu, J., He, Q., Yang, G., Zhou, W., Shao, Z. and Ni, M. (2019) Recent Advances and Prospective in Ruthenium-Based Materials for Electrochemical Water Splitting. ACS Catalysis, 9, 9973-10011. [Google Scholar] [CrossRef] 
[10] Chen, X., Wang, X., Le, J., Li, S., Wang, X., Zhang, Y., et al. (2023) Revealing the Role of Interfacial Water and Key Intermediates at Ruthenium Surfaces in the Alkaline Hydrogen Evolution Reaction. Nature Communications, 14, Article No. 5289. [Google Scholar] [CrossRef] [PubMed]
[11] Dong, K., Liang, J., Wang, Y., Zhang, L., Xu, Z., Sun, S., et al. (2022) Conductive Two-Dimensional Magnesium Metal-Organic Frameworks for High-Efficiency O2 Electroreduction to H2O2. ACS Catalysis, 12, 6092-6099. [Google Scholar] [CrossRef] 
[12] Li, T., Zhang, X., Chen, Y., Zhong, L., Li, S., Zhang, P., et al. (2021) Boosting the Water Dissociation Kinetics via Charge Redistribution of Ruthenium Decorated on S, N-Codoped Carbon. Journal of Materials Chemistry A, 9, 16967-16973. [Google Scholar] [CrossRef] 
[13] Zhu, Y.P., Guo, C., Zheng, Y. and Qiao, S. (2017) Surface and Interface Engineering of Noble-Metal-Free Electrocatalysts for Efficient Energy Conversion Processes. Accounts of Chemical Research, 50, 915-923. [Google Scholar] [CrossRef] [PubMed]
[14] Zhou, W., Jia, J., Lu, J., Yang, L., Hou, D., Li, G., et al. (2016) Recent Developments of Carbon-Based Electrocatalysts for Hydrogen Evolution Reaction. Nano Energy, 28, 29-43. [Google Scholar] [CrossRef] 
[15] Sun, X., Wu, B., Chen, J., Li, B., Cao, C., Fan, L., et al. (2023) Self-Assembly Synthesis of Ru Nanoparticles Anchored on B, N Co-Doping Carbon Support for Hydrogen Evolution: Electronic State Induced by the Strong Metal-Support Interactions. International Journal of Hydrogen Energy, 48, 9682-9689. [Google Scholar] [CrossRef] 
[16] Su, P., Pei, W., Wang, X., Ma, Y., Jiang, Q., Liang, J., et al. (2021) Exceptional Electrochemical HER Performance with Enhanced Electron Transfer between Ru Nanoparticles and Single Atoms Dispersed on a Carbon Substrate. Angewandte Chemie International Edition, 60, 16044-16050. [Google Scholar] [CrossRef] [PubMed]
[17] Liu, Z., Li, B., Feng, Y., Jia, D., Li, C. and Zhou, Y. (2022) N‐Doped Sp2/Sp3 Carbon Derived from Carbon Dots to Boost the Performance of Ruthenium for Efficient Hydrogen Evolution Reaction. Small Methods, 6, Article ID: 2200637. [Google Scholar] [CrossRef] [PubMed]
[18] Wang, J., Wei, Z., Mao, S., Li, H. and Wang, Y. (2018) Highly Uniform Ru Nanoparticles over N-Doped Carbon: pH and Temperature-Universal Hydrogen Release from Water Reduction. Energy & Environmental Science, 11, 800-806. [Google Scholar] [CrossRef] 
[19] Zhou, G., Zhang, S., Zhu, Y., Li, J., Sun, K., Pang, H., et al. (2022) Manipulating the Rectifying Contact between Ultrafine Ru Nanoclusters and N‐Doped Carbon Nanofibers for High‐Efficiency Ph‐Universal Electrocatalytic Hydrogen Evolution. Small, 19, Article ID: 2206781. [Google Scholar] [CrossRef] [PubMed]
[20] Shervedani, R.K. and Amini, A. (2015) Sulfur-Doped Graphene as a Catalyst Support: Influences of Carbon Black and Ruthenium Nanoparticles on the Hydrogen Evolution Reaction Performance. Carbon, 93, 762-773. [Google Scholar] [CrossRef]