Citation: Wenfang Peng, Shiwen Liu, Xiugang Li, Gang Feng, Jianhui Xia, Zhang-Hui Lu. Robust hydrogen production from HCOOH over amino-modified KIT-6-confined PdIr alloy nanoparticles[J]. Chinese Chemical Letters, ;2022, 33(3): 1403-1406. doi: 10.1016/j.cclet.2021.08.033 shu

Robust hydrogen production from HCOOH over amino-modified KIT-6-confined PdIr alloy nanoparticles

Wenfang Peng ^{a, b} ,
Shiwen Liu ^b ,
Xiugang Li ^a ,
Gang Feng ^c ,
Jianhui Xia ^a ,
Zhang-Hui Lu ^{a, *,}

a.
Key Laboratory of Functional Small Molecules for Ministry of Education, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China
b.
Jiangxi Provincial Center for Disease Control and Prevention, Nanchang 330029, China
c.
College of Chemistry, Nanchang University, Nanchang 330031, China

luzh@jxnu.edu.cn

Received Date: 29 June 2021
Revised Date: 31 July 2021
Accepted Date: 9 August 2021
Available Online: 12 August 2021

Figures(4)

Formic acid (FA), which can be produced via CO₂ reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH₂) lead to better catalytic activity compared to that of Pd/KIT-6-NH₂ and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h⁻¹ at ambient temperature (303 K), 100% H₂ selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH₂ can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH₂, as well as the amino-groups of KIT-6-NH₂ which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.
- Formic acid,
- Hydrogen production,
- Palladium,
- Metal nanoparticle,
- 3D mesoporous silica
1. [1]
  Y. Zhang, J. Liu, S. Li, et al., EnergyChem 1 (2019) 100021 doi: 10.1016/j.enchem.2019.100021
2. [2]
  W. Hua, H. H. Sun, F. Xu, et al., Rare Met. 39 (2020) 335-351 doi: 10.1007/s12598-020-01384-7
3. [3]
  A. Zhang, H. Du, Z. H. Lu, Acta Chim. Sin. 79 (2021) 885-902 doi: 10.6023/a21030126
4. [4]
  J. Zhang, F. Lin, L. Yang, et al., Chin. Chem. Lett. 31 (2020) 2019-2022 doi: 10.1016/j.cclet.2019.11.042
5. [5]
  X. Gu, Z. H. Lu, H. L. Jiang, et al, J. Am. Chem. Soc. 133 (2011) 11822-11825 doi: 10.1021/acs.accounts.7b00132
6. [6]
  Z. J. Zhang, Y. X. Luo, S. W. Liu, et al., J. Mater. Chem. A7 (2019) 21438-21446 doi: 10.1039/c9ta06987a
7. [7]
  Q. M. Sun, J. M. Ben, W. J. Chen, et al., Angew. Chem. Int. Ed. 59 (2020) 20183-20191 doi: 10.1002/anie.202008962
8. [8]
  Y. Yang, Z. H. Lu, Y. Hu, et al., RSC Adv. 4 (2014) 13749-13752 doi: 10.1039/C3RA47023G
9. [9]
  X. Cao, J Zhou, S. Li, et al., Rare Met. 39 (2020) 113-130 doi: 10.1007/s12598-019-01350-y
10. [10]
  L. S. Jose, M. S. Cristina, I. Svetlana, et al., Appl. Catal. B Environ. 282 (2021) 119615 doi: 10.1016/j.apcatb.2020.119615
11. [11]
  Q. Y. Bi, J. D. Lin, J. D. Liu, et al., Angew. Chem. Int. Ed. 55 (2016) 11849-11853 doi: 10.1002/anie.201605961
12. [12]
  M. Farajzadeh, H. A. lamgholiloo, F. Nasibipour, et al., Sci. Rep. 10 (2020) 18188 doi: 10.1038/s41598-020-75369-y
13. [13]
  Y. Luo, W. Nie, Y. Ding, et al., ACS Appl. Energy Mater. 4 (2021) 4945-4954 doi: 10.1021/acsaem.1c00520
14. [14]
  Y. Chao, X. F. Guo, B. Shen, et al., J. Mater. Chem. A6 (2018) 23766-23772 doi: 10.1039/C8TA09342C
15. [15]
  J. Han, Z. J. Zhang, Z. R. Hao, et al., J. Colloid Interfaces Sci. 587 (2021) 736-742 doi: 10.1016/j.jcis.2020.11.033
16. [16]
  K. Mori, S. Y. Masuda, H. Tanaka, et al., Chem. Commun. 53 (2017) 4677-4680 doi: 10.1039/C7CC00864C
17. [17]
  J. L. Santos, C. Leon, G. Monnier, et al., Int. J. Hydrog. Energy 45 (2020) 23056-23068 doi: 10.1016/j.ijhydene.2020.06.076
18. [18]
  W. Hong, M. Kitta, N. Tsumori, et al., J. Mater. Chem. A 7 (2019) 18835-18839 doi: 10.1039/c9ta06014f
19. [19]
  Z. Z. Wang, S. P. Liang, X. Y. Meng, et al., Appl. Catal. B Environ. 291 (2021) 120140 doi: 10.1016/j.apcatb.2021.120140
20. [20]
  W. Wang, X. Hong, Q. Yao, et al. J. Mater. Chem. A8 (2020) 13694-13701 doi: 10.1039/d0ta05322h
21. [21]
  C. G. Jessica, N. G. Miriam, S. T. David, et al., ACS Sustain. Chem. Eng. 8 (2020) 15030-15043 doi: 10.1021/acssuschemeng.0c05906
22. [22]
  T. Wang, J. Du, Y. Sun, et al., Chin. Chem. Lett. 32 (2021) 1186-1190 doi: 10.1016/j.cclet.2020.07.044
23. [23]
  Y. Yan, H. Li, Z. H. Lu, et al., Chin. Chem. Lett. 30 (2019) 1153-1156
24. [24]
  J. Cheng, X. Gu, X. L. Sheng, et al., J. Mater. Chem. A4 (2016) 1887 184
25. [25]
  K. Wang, Q. Yao, Q. Qing, et al., J. Mater. Chem. A7 (2019) 9903-9911 doi: 10.1039/c9ta01066a
26. [26]
  I. Choi, H. Lee, G. Lee, et al., Rare Met. 39 (2020) 767-783 doi: 10.1007/s12598-019-01203-8
27. [27]
  Z. Pan, Z. Tang, Y. Zhang, et al., Tungsten 2 (2020) 390-402 doi: 10.1007/s42864-020-00065-3
28. [28]
  Z. Zhang, S. Zhang, Q. Yao, et al., Inorg. Chem. Front. 5 (2018) 370-377 doi: 10.1039/C7QI00555E
29. [29]
  K. Zhan, P. Liu, J. Dong, et al., Chin. Chem. Lett. 31 (2020) 1630-1634
30. [30]
  X. Ji, K. T. Lee, R. Holden, et al., Nat. Chem. 2 (2010) 286-293 doi: 10.1002/adma.201703038
31. [31]
  F. Z. Song, Q. L. Zhu, X. C. Yang, et al., Adv. Energy Mater. 8 (2017) 1701416
32. [32]
  F. Q. Tang, L. L. Li, D. Chen, Adv. Mater. 24 (2012) 1504-1534 doi: 10.1039/c9ta10196a
33. [33]
  Q. J. Wang, N. Tsumori, M. Kitta, et al., ACS Catal. 8 (2018) 12041-12045 doi: 10.1021/acscatal.8b03444
34. [34]
  G. X. Yang, Y. Kuwahara, S. Masuda, et al., J. Mater. Chem. A8 (2020) 4437-4446 doi: 10.1021/ja200122f
35. [35]
  X. Li, A. E. Surkus, J. Rabeah, et al., Angew. Chem. Int. Ed. 59 (2020) 15849-15854 doi: 10.1002/anie.202004125
36. [36]
  A. B. Redondo, F. L. Morel, M. Ranocchiari, et al., ACS Catal. 5 (2015) 7099-7103 doi: 10.1021/acscatal.5b01987
37. [37]
  G. D. Feng, J. Y. Wang, M. Boronat, et al., J. Am. Chem. Soc. 140 (2018) 4770-4773 doi: 10.1021/jacs.8b00093
38. [38]
  Y. D. Zou, B. T. Huang, L. H. Cao, et al., Adv. Mater. 33 (2020) 2005215
39. [39]
  J. Liang, Z. B. Liang, R. Q. Zou, et al., Adv. Mater. 29 (2017) 1701139 doi: 10.1002/adma.201701139
40. [40]
  S. Masuda, K. Mori, Y. Futamura, et al., ACS Catal. 8 (2018) 2277-2285 doi: 10.1021/acscatal.7b04099
41. [41]
  M. Huang, Q. Yao, G. Feng, et al., Inorg. Chem. 59 (2020) 5781-5790 doi: 10.1021/acs.inorgchem.0c00600
42. [42]
  K. Koh, M. Jeon, C. W. Yoon, et al., J. Mater. Chem. A5 (2017) 16150-16161 doi: 10.1039/C7TA02040F
43. [43]
  Y. X. Luo, Q. F. Yang, W. D. Nie, et al., ACS Appl. Mater. Interfaces 12 (2020) 8082-8090 doi: 10.1021/acsami.9b16981
44. [44]
  W. D. Nie, Y. X. Luo, Q. F. Yang, et al., Inorg. Chem. Front. 7 (2020) 709-717 doi: 10.1039/c9qi01375j
45. [45]
  S. P. Wang, S. H. Hou, C. Wu, et al., Chin. Chem. Lett. 30 (2019) 398-402
1. [1]
  Yiyue Ding , Qiuxiang Zhang , Lei Zhang , Qilu Yao , Gang Feng , Zhang-Hui Lu . Exceptional activity of amino-modified rGO-immobilized PdAu nanoclusters for visible light-promoted dehydrogenation of formic acid. Chinese Chemical Letters, 2024, 35(7): 109593-. doi: 10.1016/j.cclet.2024.109593
2. [2]
  Tianhao Li , Wenguang Tu , Zhigang Zou . In situ photocatalytically enhanced thermogalvanic cells for electricity and hydrogen production. Chinese Journal of Structural Chemistry, 2024, 43(1): 100195-100195. doi: 10.1016/j.cjsc.2023.100195
3. [3]
  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
4. [4]
  Xinlong Zheng , Zhongyun Shao , Jiaxin Lin , Qizhi Gao , Zongxian Ma , Yiming Song , Zhen Chen , Xiaodong Shi , Jing Li , Weifeng Liu , Xinlong Tian , Yuhao Liu . Recent advances of CuSbS₂ and CuPbSbS₃ as photocatalyst in the application of photocatalytic hydrogen evolution and degradation. Chinese Chemical Letters, 2025, 36(3): 110533-. doi: 10.1016/j.cclet.2024.110533
5. [5]
  Hailong He , Wenbing Wang , Wenmin Pang , Chen Zou , Dan Peng . Double stimulus-responsive palladium catalysts for ethylene polymerization and copolymerization. Chinese Chemical Letters, 2024, 35(7): 109534-. doi: 10.1016/j.cclet.2024.109534
6. [6]
  Junlong Tang , Yuhan Zhao , Yangbin Jin , Liren Zhang , Yuanfang Wang , Wanqing Wu , Huanfeng Jiang . Palladium-catalyzed modular biomimetic synthesis of lignans derivatives. Chinese Chemical Letters, 2025, 36(7): 110969-. doi: 10.1016/j.cclet.2025.110969
7. [7]
  Zhao Gu , Yunhui Yang , Song Ye , Congyang Wang . 2,3-Arylacylation of allenes through synergetic catalysis of palladium and N-heterocyclic carbene. Chinese Chemical Letters, 2025, 36(5): 110334-. doi: 10.1016/j.cclet.2024.110334
8. [8]
  Xiaohui Fu , Yanping Zhang , Juan Liao , Zhen-Hua Wang , Yong You , Jian-Qiang Zhao , Mingqiang Zhou , Wei-Cheng Yuan . Palladium-catalyzed enantioselective decarboxylation of vinyl cyclic carbamates: Generation of amide-based aza-1,3-dipoles and application to asymmetric 1,3-dipolar cycloaddition. Chinese Chemical Letters, 2024, 35(12): 109688-. doi: 10.1016/j.cclet.2024.109688
9. [9]
  Xiao Liu , Hangqi Liu , Qian Wang , Dandan Zheng , Sibo Wang , Masakazu Anpo , Guigang Zhang . Rational synthesis of poly(heptazine imides) nanorod in ternary LiCl/NaCl/KCl for visible light hydrogen production. Chinese Chemical Letters, 2025, 36(12): 111621-. doi: 10.1016/j.cclet.2025.111621
10. [10]
  Miaosen Yang , Junyang Ding , Zhiwei Wang , Jingwen Zhang , Zimo Peng , Xijun Liu . NiMo-based alloy and its sulfides for energy-saving hydrogen production via sulfion oxidation assisted alkaline seawater splitting. Chinese Chemical Letters, 2025, 36(9): 110861-. doi: 10.1016/j.cclet.2025.110861
11. [11]
  Wengao Zeng , Yuchen Dong , Xiaoyuan Ye , Ziying Zhang , Tuo Zhang , Xiangjiu Guan , Liejin Guo . Crystalline carbon nitride with in-plane built-in electric field accelerates carrier separation for excellent photocatalytic hydrogen evolution. Chinese Chemical Letters, 2024, 35(4): 109252-. doi: 10.1016/j.cclet.2023.109252
12. [12]
  Hao-Nan Zhou , Lan-Yan Li , Hong-Bing Mo , Yi-Xin Li , Jun Yan , Chao Liu . Ligand-engineered octanuclear bismuth-oxo clusters with exposed active sites for enhanced CO₂-to-HCOOH electroreduction. Chinese Chemical Letters, 2025, 36(10): 111269-. doi: 10.1016/j.cclet.2025.111269
13. [13]
  Peng Jin , Sili Lin , Dongmei Wang , Jinsong Fan , Qingyun Liu , Kun Li . Valence-band hybridization endows the reaction specificity of AgPd nanozyme for exclusive peroxidase mimicking and improved sensing performance. Chinese Chemical Letters, 2025, 36(11): 110916-. doi: 10.1016/j.cclet.2025.110916
14. [14]
  Xiaoke Xi , Xinpeng Li , Yang Liu , Yucheng Zhang , Linmei Li , Jianming Li , Xu Jin , Shuhong Jiao , Zhanwu Lei , Ruiguo Cao . Monolithic medium-entropy alloy electrode enables efficient and stable oxygen evolution reaction. Chinese Chemical Letters, 2025, 36(12): 110535-. doi: 10.1016/j.cclet.2024.110535
15. [15]
  Jiawei Hu , Kai Xia , Ao Yang , Zhihao Zhang , Wen Xiao , Chao Liu , Qinfang Zhang . Interfacial Engineering of Ultrathin 2D/2D NiPS₃/C₃N₅ Heterojunctions for Boosting Photocatalytic H₂ Evolution. Acta Physico-Chimica Sinica, 2024, 40(5): 2305043-0. doi: 10.3866/PKU.WHXB202305043
16. [16]
  Shuang Cao , Bo Zhong , Chuanbiao Bie , Bei Cheng , Feiyan Xu . Insights into Photocatalytic Mechanism of H₂ Production Integrated with Organic Transformation over WO₃/Zn_0.5Cd_0.5S S-Scheme Heterojunction. Acta Physico-Chimica Sinica, 2024, 40(5): 2307016-0. doi: 10.3866/PKU.WHXB202307016
17. [17]
  Jiangping Chen , Hongju Ren , Kai Wu , Huihuang Fang , Chongqi Chen , Li Lin , Yu Luo , Lilong Jiang . Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces. Chinese Journal of Structural Chemistry, 2024, 43(2): 100236-100236. doi: 10.1016/j.cjsc.2024.100236
18. [18]
  Peiyang Du , Ling Yuan , Tong Bao , Yamin Xi , Jiaxin Li , Yin Bi , Luli Yin , Jing Wang , Chao Liu . Facet effect of metal-organic frameworks on supporting co-catalysts for photocatalytic hydrogen peroxide production. Chinese Chemical Letters, 2025, 36(11): 110472-. doi: 10.1016/j.cclet.2024.110472
19. [19]
  Run Chai , Qiujie Wu , Yongchao Liu , Xiaohui Song , Xuyong Feng , Yi Sun , Hongfa Xiang . A 3D dual layer host with enhanced sodiophilicity as stable anode for high-energy sodium metal batteries. Chinese Chemical Letters, 2025, 36(6): 110007-. doi: 10.1016/j.cclet.2024.110007
20. [20]
  Huipeng Zhao , Xiaoqiang Du . Polyoxometalates as the redox anolyte for efficient conversion of biomass to formic acid. Chinese Journal of Structural Chemistry, 2024, 43(2): 100246-100246. doi: 10.1016/j.cjsc.2024.100246

Get Citation

PDF

XML

Metrics

PDF Downloads(6)
Abstract views(1528)
HTML views(205)

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