Citation: Xuyun Gao, Bo Li, Xuzhuo Sun, Baofan Wu, Yanping Hu, Zhichao Ning, Jun Li, Ning Wang. Engineering heterostructure and crystallinity of Ru/RuS₂ nanoparticle composited with N-doped graphene as electrocatalysts for alkaline hydrogen evolution[J]. Chinese Chemical Letters, ;2021, 32(11): 3591-3595. doi: 10.1016/j.cclet.2021.03.053 shu

Engineering heterostructure and crystallinity of Ru/RuS₂ nanoparticle composited with N-doped graphene as electrocatalysts for alkaline hydrogen evolution

Xuyun Gao ^{a, b, 1} ,
Bo Li ^{a, 1} ,
Xuzhuo Sun ^{a, *,} ,
Baofan Wu ^a ,
Yanping Hu ^b ,
Zhichao Ning ^a ,
Jun Li ^{b, *,} ,
Ning Wang ^{b, *,}

a.
College of Chemistry and Chemical Engineering, Henan University of Technology, Zhengzhou 450001, China
b.
Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry & Materials Science, Northwest University, Xi'an 710069, China

sunxuzhuo@haut.edu.cn

junli@nwu.edu.cn

ningwang@nwu.edu.cn

Received Date: 20 February 2021
Revised Date: 19 March 2021
Accepted Date: 22 March 2021
Available Online: 23 March 2021

Figures(5)

Crystalline engineering and heterostructure have attracted much attention as effective strategies to improve the electrocatalytic activity for hydrogen evolution reaction (HER). In this study, a new heterostructure catalyst (Ru/RuS₂@N-rGO) with low crystallinity was fabricated by a simple and low-temperature method for HER in alkaline solution, applying the Na₂SO₄ as S source and polypyrrole as N source. Optimizing through the controllable crystalline engineering and composition ratio of Ru and RuS₂, the Ru/RuS₂@N-rGO heterocatalyst at the calcining 500 ℃ revealed highly efficient HER activity with overpotential 18 mV at a current density 10 mA/cm² and remarkable stability for 24 h in 1.0 mol/L KOH. This work provides a facile and effective method in designing advanced electrocatalysts for HER in the alkaline electrolytes by synergistically structural and component modulations.
- Low crystallinity,
- Ru/RuS₂ heterostructure,
- Graphene,
- Electrocatalytic hydrogen evolution,
- Alkaline solution
1. [1]
  S. Chu, A. Majumdar, Nature 488 (2012) 294-303. doi: 10.1038/nature11475
2. [2]
  J.A. Turner, Science 305 (2004) 972-974. doi: 10.1126/science.1103197
3. [3]
  Y.F. Yu, Y.M. Shi, B. Zhang, Acc. Chem. Res. 51 (2018) 1711-1721. doi: 10.1021/acs.accounts.8b00193
4. [4]
  X. Wang, Q.X. Li, P.H. Shi, et al., Small 15 (2019) 1901530. doi: 10.1002/smll.201901530
5. [5]
  X. Ding, L.L. Zhang, Y. Wang, A.H. Liu, Y. Gao, Coord. Chem. Rev. 357 (2018) 130-143. doi: 10.1016/j.ccr.2017.10.020
6. [6]
  T. Liu, P. Li, N. Yao, et al., Angew. Chem. Int. Ed. 58 (2019) 4679-4684. doi: 10.1002/anie.201901409
7. [7]
  G. Huang, Z.H. Xiao, R. Chen, S.G. Wang, ACS Sustain. Chem. Eng. 6 (2018) 15954-15969. doi: 10.1021/acssuschemeng.8b04397
8. [8]
  Y. Jiao, Y. Zheng, M. Jaroniec, S.Z. Qiao, Chem. Soc. Rev. 44 (2015) 2060-2086. doi: 10.1039/C4CS00470A
9. [9]
  K.D. Xia, J.P. Guo, C.J. Xuan, T. Huang, Z.P. Deng, Chin. Chem. Lett. 30 (2020) 192-196. doi: 10.1109/msp.2020.3018085
10. [10]
  Y.M. Zhao, H.J. Cong, W. Luo, et al., Angew. Chem. Int. Ed. 60 (2021) 1-6. doi: 10.1002/anie.202015604
11. [11]
  K.D. Li, J.F. Zhang, R. Wu, Y.F. Yu, B. Zhang, Adv. Sci. 3 (2016) 1500426. doi: 10.1002/advs.201500426
12. [12]
  N. Mahmood, Y.D. Yao, J.W. Zhang, et al., Adv. Sci. 5 (2018) 1700464. doi: 10.1002/advs.201700464
13. [13]
  F. Safizadeh, E. Ghali, G. Houlachi, Int. J. Hydrogen Energy 40 (2015) 256-274. doi: 10.1016/j.ijhydene.2014.10.109
14. [14]
  J.M. Wei, M. Zhou, A.C. Long, et al., Nano-micro Lett. 10 (2018) 75. doi: 10.1007/s40820-018-0229-x
15. [15]
  J.L. Liu, Y. Zheng, D.D. Zhu, et al., Nanoscale 9 (2017) 16616-16621. doi: 10.1039/C7NR06111K
16. [16]
  B.Y. Lu, L. Guo, F. Wu, et al., Nat. Commun. 10 (2019) 631. doi: 10.1038/s41467-019-08419-3
17. [17]
  R. Subbaraman, D. Tripkovic, D. Strmcnik, et al., Science 334 (2011) 1256-1260. doi: 10.1126/science.1211934
18. [18]
  R. Boppella, J.W. Tan, W. Yang, J. Moon, Adv. Funct. Mater. 29 (2018) 1807976. doi: 10.1002/adfm.201807976
19. [19]
  X.Y. Gao, J. Chen, X.Z. Sun, et al., ACS Appl. Nano Mater. 3 (2020) 12269-12277. doi: 10.1021/acsanm.0c02739
20. [20]
  Z.J. Sun, Y. Liang, Y.M. Wu, Y.F. Yu, B. Zhang, ACS Sustain. Chem. Eng. 6 (2018) 11206-11210. doi: 10.1021/acssuschemeng.8b02676
21. [21]
  J.X. Diao, Y. Qiu, S.Q. Liu, et al., Adv. Mater. 32 (2019) 905679.
22. [22]
  X.L. Jiang, H. Jang, S.G. Liu, et al., Angew. Chem. Int. Ed. 60 (2021) 4110-4116. doi: 10.1002/anie.202014411
23. [23]
  S. Higgins, Nat. Chem. 2 (2010) 1100-1100. doi: 10.1038/nchem.917
24. [24]
  Y.T. Li, L.A. Zhang, Y. Qin, et al., ACS Catal. 8 (2018) 5714-5720. doi: 10.1021/acscatal.8b01609
25. [25]
  J. Yu, Q.J. He, G.M. Yang, et al., ACS Catal. 9 (2019) 9973-10011. doi: 10.1021/acscatal.9b02457
26. [26]
  Y. Zheng, Y. Jiao, Y.H. Zhu, et al., J. Am. Chem. Soc. 138 (2016) 16174-16181. doi: 10.1021/jacs.6b11291
27. [27]
  W.D. Li, Y.A. Liu, M. Wu, et al., Adv. Mater. 30 (2018) 1800676. doi: 10.1002/adma.201800676
28. [28]
  J.W. Liu, G.Z. Ding, J.Y. Yu, et al., J. Mater. Chem. A Mater. Energy Sustain. 7 (2019) 18072-18080. doi: 10.1039/C9TA06206H
29. [29]
  Z.K. Peng, H.Y. Wang, L.L. Zhou, et al., J. Mater. Chem. A Mater. Energy Sustain. 7 (2019) 6676-6685. doi: 10.1039/C8TA09136F
30. [30]
  X.Z. Sun, X.Y. Gao, J. Chen, et al., ACS Appl. Mater. Interfaces 12 (2020) 48591-48597. doi: 10.1021/acsami.0c14170
31. [31]
  M. Tan, Y. Wang, A. Taguchi, et al., Int. J. Hydrogen Energy 44 (2019) 7320-7325. doi: 10.1016/j.ijhydene.2019.01.245
32. [32]
  S.H. Ye, F.Y. Luo, T.T. Xu, et al., Nano Energy 68 (2020) 104301. doi: 10.1016/j.nanoen.2019.104301
33. [33]
  X.L. Chen, J. Zheng, X. Zhong, et al., Catal. Sci. Technol. 7 (2017) 4964-4970. doi: 10.1039/C7CY01539A
34. [34]
  W.Y. Gou, J.Y. Li, W. Gao, et al., ChemCatChem 11 (2019) 1970-1976. doi: 10.1002/cctc.201900006
35. [35]
  X.K. Kong, K. Xu, C.G. Zhang, et al., ACS Catal. 6 (2016) 1487-1492. doi: 10.1021/acscatal.5b02730
36. [36]
  D. Luo, B.Y. Zhou, Z.X. Li, et al., J. Mater. Chem. A Mater. Energy Sustain. 6 (2018) 2311-2317. doi: 10.1039/C7TA09493K
37. [37]
  W. Luo, L.B. Li, N. Yao, F.L. Yang, G.Z. Cheng, ACS Catal. 10 (2020) 73322-77327.
38. [38]
  Y. Peng, B.Z. Lu, L.M. Chen, et al., J. Mater. Chem. A Mater. Energy Sustain. 5 (2017) 18261-18269. doi: 10.1039/C7TA03826G
39. [39]
  J. Wang, Z.Z. Wei, S.J. Mao, H.R. Li, Y. Wang, Energy Environ. Sci. 11 (2018) 800-806. doi: 10.1039/C7EE03345A
40. [40]
  J. Yu, Y.N. Guo, S.S. Miao, et al., ACS Appl. Mater. Interfaces 10 (2018) 34098-34107. doi: 10.1021/acsami.8b08239
41. [41]
  J.Y. Yu, Y.S. Yang, R.T. Jia, et al., Appl. Surf. Sci. 529 (2020) 147080. doi: 10.1016/j.apsusc.2020.147080
42. [42]
  U. Joshi, S. Malkhandi, Y. Ren, et al., ACS Appl. Mater. Interfaces 10 (2018) 6354-6360. doi: 10.1021/acsami.7b17970
43. [43]
  P.S. Li, X.X. Duan, S.Y. Wang, et al., Small 15 (2019) 1904043. doi: 10.1002/smll.201904043
44. [44]
  Y. Li, J.W. Li, J.X. Chen, et al., J. Power Sources 472 (2020) 228625. doi: 10.1016/j.jpowsour.2020.228625
45. [45]
  Y.J. Xia, W.Q. Wu, H. Wang, et al., Nanotechnology 31 (2020) 145401. doi: 10.1088/1361-6528/ab62d3
46. [46]
  Y.L. Zhu, H.A. Tahini, Y. Wang, et al., J. Mater. Chem. A Mater. Energy Sustain. 7 (2019) 14222-14232. doi: 10.1039/C9TA04120F
47. [47]
  J.W. Zhu, Y. Guo, F. Liu, et al., Angew. Chem. Int. Ed. 60 (2021) 12328-12334. doi: 10.1002/anie.202101539
48. [48]
  Y.P. Li, Y.F. Yu, Y.F. Huang, et al., ACS Catal. 5 (2014) 448-455. doi: 10.1021/cs501635v
49. [49]
  M. Zhao, Y.F. Wu, W.W. Cai, et al., Int. J. Hydrogen Energy 44 (2019) 31053-31061. doi: 10.1016/j.ijhydene.2019.10.023
50. [50]
  X.Y. Zhang, T. Guo, T.Y. Liu, et al., Electrochim. Acta 323 (2019) 134798. doi: 10.1016/j.electacta.2019.134798
51. [51]
  C. Zhang, Y.M. Shi, Y.F. Yu, Y.H. Yu, B. Zhang, ACS Catal. 8 (2018) 8077-8083. doi: 10.1021/acscatal.8b02056
52. [52]
  H.H. Sun, X.Y. Ji, Y.F. Qiu, et al., J. Alloys. Compd. 777 (2019) 514-523. doi: 10.1016/j.jallcom.2018.10.364
53. [53]
  J. Kibsgaard, Z.B. Chen, B.N. Reinecke, T.F. Jaramillo, Nat. Mater. 11 (2012) 963-969. doi: 10.1038/nmat3439
54. [54]
  C. Sun, P.P. Wang, H. Wang, et al., Nano Res. 12 (2019) 1613-1618. doi: 10.1007/s12274-019-2400-1
55. [55]
  H. Wang, X. Xiao, S.Y. Liu, et al., J. Am. Chem. Soc. 141 (2019) 18578-18584. doi: 10.1021/jacs.9b09932
56. [56]
  X. Wang, Y.W. Zhang, H.N. Si, et al., J. Am. Chem. Soc. 142 (2020) 4298-4308. doi: 10.1021/jacs.9b12113
57. [57]
  J.F. Xie, J.J. Zhang, S. Li, et al., J. Am. Chem. Soc. 135 (2013) 17881-17888. doi: 10.1021/ja408329q
1. [1]
  Caili Yang , Tao Long , Ruotong Li , Chunyang Wu , Yuan-Li Ding . Pseudocapacitance dominated Li₃VO₄ encapsulated in N-doped graphene via 2D nanospace confined synthesis for superior lithium ion capacitors. Chinese Chemical Letters, 2025, 36(2): 109675-. doi: 10.1016/j.cclet.2024.109675
2. [2]
  Cheng Guo , Xiaoxiao Zhang , Xiujuan Hong , Yiqiu Hu , Lingna Mao , Kezhi Jiang . Graphene as adsorbent for highly efficient extraction of modified nucleosides in urine prior to liquid chromatography-tandem mass spectrometry analysis. Chinese Chemical Letters, 2024, 35(4): 108867-. doi: 10.1016/j.cclet.2023.108867
3. [3]
  Chaozheng He , Pei Shi , Donglin Pang , Zhanying Zhang , Long Lin , Yingchun Ding . First-principles study of the relationship between the formation of single atom catalysts and lattice thermal conductivity. Chinese Chemical Letters, 2024, 35(6): 109116-. doi: 10.1016/j.cclet.2023.109116
4. [4]
  Haibin Yang , Duowen Ma , Yang Li , Qinghe Zhao , Feng Pan , Shisheng Zheng , Zirui Lou . Mo doped Ru-based cluster to promote alkaline hydrogen evolution with ultra-low Ru loading. Chinese Journal of Structural Chemistry, 2023, 42(11): 100031-100031. doi: 10.1016/j.cjsc.2023.100031
5. [5]
  Tian TIAN , Meng ZHOU , Jiale WEI , Yize LIU , Yifan MO , Yuhan YE , Wenzhi JIA , Bin HE . Ru-doped Co₃O₄/reduced graphene oxide: Preparation and electrocatalytic oxygen evolution property. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 385-394. doi: 10.11862/CJIC.20240298
6. [6]
  Minying Wu , Xueliang Fan , Wenbiao Zhang , Bin Chen , Tong Ye , Qian Zhang , Yuanyuan Fang , Yajun Wang , Yi Tang . Highly dispersed Ru nanospecies on N-doped carbon/MXene composite for highly efficient alkaline hydrogen evolution. Chinese Chemical Letters, 2024, 35(4): 109258-. doi: 10.1016/j.cclet.2023.109258
7. [7]
  Ping Wang , Ting Wang , Ming Xu , Ze Gao , Hongyu Li , Bowen Li , Yuqi Wang , Chaoqun Qu , Ming Feng . Keplerate polyoxomolybdate nanoball mediated controllable preparation of metal-doped molybdenum disulfide for electrocatalytic hydrogen evolution in acidic and alkaline media. Chinese Chemical Letters, 2024, 35(7): 108930-. doi: 10.1016/j.cclet.2023.108930
8. [8]
  Jing Cao , Dezheng Zhang , Bianqing Ren , Ping Song , Weilin Xu . Mn incorporated RuO₂ nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline. Chinese Chemical Letters, 2024, 35(10): 109863-. doi: 10.1016/j.cclet.2024.109863
9. [9]
  Guoliang Gao , Guangzhen Zhao , Guang Zhu , Bowen Sun , Zixu Sun , Shunli Li , Ya-Qian Lan . Recent advancements in noble-metal electrocatalysts for alkaline hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(1): 109557-. doi: 10.1016/j.cclet.2024.109557
10. [10]
  Qiang Cao , Xue-Feng Cheng , Jia Wang , Chang Zhou , Liu-Jun Yang , Guan Wang , Dong-Yun Chen , Jing-Hui He , Jian-Mei Lu . Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol. Chinese Chemical Letters, 2024, 35(4): 108759-. doi: 10.1016/j.cclet.2023.108759
11. [11]
  Bowen Li , Ting Wang , Ming Xu , Yuqi Wang , Zhaoxing Li , Mei Liu , Wenjing Zhang , Ming Feng . Structuring MoO₃-polyoxometalate hybrid superstructures to boost electrocatalytic hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(2): 110467-. doi: 10.1016/j.cclet.2024.110467
12. [12]
  Junan Pan , Xinyi Liu , Huachao Ji , Yanwei Zhu , Yanling Zhuang , Kang Chen , Ning Sun , Yongqi Liu , Yunchao Lei , Kun Wang , Bao Zang , Longlu Wang . The strategies to improve TMDs represented by MoS₂ electrocatalytic oxygen evolution reaction. Chinese Chemical Letters, 2024, 35(11): 109515-. doi: 10.1016/j.cclet.2024.109515
13. [13]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
14. [14]
  Jie Zhou , Chuanxiang Zhang , Changchun Hu , Shuo Li , Yuan Liu , Zhu Chen , Song Li , Hui Chen , Rokayya Sami , Yan Deng . Electrochemical aptasensor based on black phosphorus-porous graphene nanocomposites for high-performance detection of Hg²⁺. Chinese Chemical Letters, 2024, 35(11): 109561-. doi: 10.1016/j.cclet.2024.109561
15. [15]
  Xin Wang , Changzhao Chen , Qishen Wang , Kai Dai . Graphene quantum dot modified Bi2MoO6 nanoflower for efficient degradation of BPA under visible light. Chinese Journal of Structural Chemistry, 2024, 43(12): 100473-100473. doi: 10.1016/j.cjsc.2024.100473
16. [16]
  Xiangyuan Zhao , Jinjin Wang , Jinzhao Kang , Xiaomei Wang , Hong Yu , Cheng-Feng Du . Ni nanoparticles anchoring on vacuum treated Mo2TiC2Tx MXene for enhanced hydrogen evolution activity. Chinese Journal of Structural Chemistry, 2023, 42(10): 100159-100159. doi: 10.1016/j.cjsc.2023.100159
17. [17]
  Jiao Li , Chenyang Zhang , Chuhan Wu , Yan Liu , Xuejian Zhang , Xiao Li , Yongtao Li , Jing Sun , Zhongmin Su . Defined organic-octamolybdate crystalline superstructures derived Mo₂C@C as efficient hydrogen evolution electrocatalysts. Chinese Chemical Letters, 2024, 35(6): 108782-. doi: 10.1016/j.cclet.2023.108782
18. [18]
  Bin Dong , Ning Yu , Qiu-Yue Wang , Jing-Ke Ren , Xin-Yu Zhang , Zhi-Jie Zhang , Ruo-Yao Fan , Da-Peng Liu , Yong-Ming Chai . Double active sites promoting hydrogen evolution activity and stability of CoRuOH/Co₂P by rapid hydrolysis. Chinese Chemical Letters, 2024, 35(7): 109221-. doi: 10.1016/j.cclet.2023.109221
19. [19]
  Zhi Zhu , Xiaohan Xing , Qi Qi , Wenjing Shen , Hongyue Wu , Dongyi Li , Binrong Li , Jialin Liang , Xu Tang , Jun Zhao , Hongping Li , Pengwei Huo . Fabrication of graphene modified CeO2/g-C3N4 heterostructures for photocatalytic degradation of organic pollutants. Chinese Journal of Structural Chemistry, 2023, 42(12): 100194-100194. doi: 10.1016/j.cjsc.2023.100194
20. [20]
  Ying Chen , Xingyuan Xia , Lei Tian , Mengying Yin , Ling-Ling Zheng , Qian Fu , Daishe Wu , Jian-Ping Zou . Constructing built-in electric field via CuO/NiO heterojunction for electrocatalytic reduction of nitrate at low concentrations to ammonia. Chinese Chemical Letters, 2024, 35(12): 109789-. doi: 10.1016/j.cclet.2024.109789

Get Citation

PDF

XML

Metrics

PDF Downloads(11)
Abstract views(628)
HTML views(140)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Engineering heterostructure and crystallinity of Ru/RuS2 nanoparticle composited with N-doped graphene as electrocatalysts for alkaline hydrogen evolution

Metrics

通讯作者: 陈斌, bchen63@163.com

Engineering heterostructure and crystallinity of Ru/RuS₂ nanoparticle composited with N-doped graphene as electrocatalysts for alkaline hydrogen evolution