Citation: Haoyu Sun, Dun Li, Yuanyuan Min, Yingying Wang, Yanyun Ma, Yiqun Zheng, Hongwen Huang. 多级钯-铜-银多孔纳米花作为高效电催化剂催化CO₂还原为C₂₊产物[J]. Acta Physico-Chimica Sinica, ;2024, 40(6): 230700. doi: 10.3866/PKU.WHXB202307007 shu

多级钯-铜-银多孔纳米花作为高效电催化剂催化CO₂还原为C₂₊产物

Haoyu Sun ¹ ,
Dun Li ² ,
Yuanyuan Min ¹ ,
Yingying Wang ^3,, ,
Yanyun Ma ⁴ ,
Yiqun Zheng ^1,, ,
Hongwen Huang ^2,,

1.
School of Chemistry, Chemical Engineering, and Materials, Jining University, Qufu 273155, Shandong Province, China;
2.
College of Materials Science and Engineering, Hunan University, Changsha 410082, China;
3.
Health Management Department, Shandong Vocational College of Light Industry, Zibo 255300, Shandong Province, China;
4.
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, Jiangsu Province, China

Corresponding author: Yingying Wang, Yiqun Zheng, Hongwen Huang,
Received Date: 3 July 2023
Revised Date: 14 August 2023
Accepted Date: 19 August 2023

Fund Project: This work was financially supported by the Natural Science Foundation of China (21701100), Shandong Provincial Natural Science Foundation, China (2020MB048, ZR2022MB120), Young Innovative Talents Introduction & Cultivation Program for Colleges and Universities of Shandong Province, China (Granted by Department of Education of Shandong Province, Sub-Title: Innovative Research Team on Energy Storage and Environment Materials), the University Feature Laboratory for Energy Conversion and Nanocatalysis of Shandong Province, Doctoral Startup Research Funding, China (2020BSZX01) and Hundred Outstanding Talent Program of Jining University, China (2020ZYRC05). This work is also supported by Suzhou Key Laboratory of Functional Nano & Soft Materials, Collaborative Innovation Center of Suzhou Nano Science & Technology, the 111 Project, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, China.

近年来，具有可控元素分布的铜基多金属纳米晶作为CO₂还原反应（CO₂RR）的电催化剂，受到了广泛研究。通过对铜电催化剂进行二次甚至多次的金属元素修饰，能够有效改变其整体d带结构并引起d带中心的位移。这种变化可以影响铜对关键中间体的表面亲和力，从而影响后续的催化途径。除了调整电子结构，形貌工程也成为提高CO₂RR电催化性能的有效手段。相对于随机形状的球形颗粒，基于二维纳米片构建的三维多孔结构有利于最大限度地暴露表面原子，为催化过程中产生的关键中间体提供丰富的扩散通道和反应中心。然而，通过设计合成路线构建这种类型的纳米结构是一项技术挑战，传统的分步自组装策略耗时且难以精确控制结构。因此，我们的研究旨在实现高纯度的合成方法，制备这种独特的纳米结构，并精确调控元素组成和电子结构，以探索结构优势与CO₂RR电化学性能改善之间的潜在关系，具有重要的应用价值。在此研究中，我们合理设计了钯-铜-银（Pd-Cu-Ag）纳米晶的二维-三维杂化结构，实现了可控的合成过程，并验证了其在电化学CO₂还原中的应用潜力。合成过程中，通过使用封装剂十八烷基三甲基氯化铵，成功地将Au@Cu_xO纳米球转化为层状CuAg纳米花（HNFs）。有趣的是，该过程中原位形成了作为构建单元的纳米薄片。通过对CuAg HNFs与Na₂PdCl₄进行电偶置换，除去了Ag和Cu，引入了零价的Pd，并在纳米片上形成了大量孔隙。我们对这些CuAg电催化剂进行了CO₂RR测试，结果显示Pd_0.7Cu_40.0Ag_59.7PHNs在C₂₊产物选择性（69.5%）和C₂₊分电流密度（-349.1 mA·cm^-2）方面表现出最佳性能。密度泛函理论（DFT）模拟表明，PdAgCu表面具有独特的电子性质，降低了C-C偶联反应的能垒，凸显了Pd掺杂对CuAg电催化剂CO₂还原的卓越性能。本研究为基于多孔纳米薄片构建多层次多金属纳米结构提供了一种直观方法，并验证了其在电催化方面的结构优势，为高效的CO₂RR催化剂的合理设计提供了依据。
- CO₂ electroreduction,
- Noble metal,
- Porous,
- Hierarchical structures,
- C₂₊ products
1. [1]
  (1) Xia, W.; Xie, Y.; Jia, S.; Han, S.; Qi, R.; Chen, T.; Xing, X.; Yao, T.; Zhou, D.; Dong, X.; et al. J. Am. Chem. Soc. 2023, 145, 17253. doi:10.1021/jacs.3c04612
2. [2]
  (2) Xue, H.; Zhao, Z.; Liao, P.; Chen, X. J. Am. Chem. Soc. 2023, 145, 14978. doi:10.1021/jacs.3c05023
3. [3]
  (3) Bi, J.; Li, P.; Liu, J.; Wang, Y.; Song, X.; Kang, X.; Sun, X.; Zhu, Q.; Han, B. Angew. Chem. Int. Ed. 2023, 1, e202307612. doi:10.1002/anie.202307612
4. [4]
  (4) Ling, N.; Zhang, J.; Wang, M.; Wang, Z.; Mi, Z.; Bin Dolmanan, S.; Zhang, M.; Wang, B.; Leow, W. R.; Zhang, J.; et al. Angew. Chem. Int. Ed. 2023, 1, e202308782. doi:10.1002/anie.202308782
5. [5]
  (5) Weng, S.; Toh, W. L.; Surendranath, Y. J. Am. Chem. Soc. 2023, 145, 16787. doi:10.1021/jacs.3c04769
6. [6]
  (6) Jia, H.; Yang, Y.; Chow, T. H.; Zhang, H.; Liu, X.; Wang, J.; Zhang, C. Adv. Funct. Mater. 2021, 31, 2101255. doi:10.1002/adfm.202101255
7. [7]
  (7) Zheng, Y.; Zhang, J.; Ma, Z.; Zhang, G.; Zhang, H.; Fu, X.; Ma, Y.; Liu, F.; Liu, M.; Huang, H. Small 2022, 18, e2201695. doi:10.1002/small.202201695
8. [8]
  (8) Kuhn, A. N.; Zhao, H.; Nwabara, U. O.; Lu, X.; Liu, M.; Pan, Y. T.; Zhu, W.; Kenis, P. J. A.; Yang, H. Adv. Funct. Mater. 2021, 31, 2101668. doi:10.1002/adfm.202101668
9. [9]
  (9) Wei, D.; Wang, Y.; Dong, C. L.; Zhang, Z.; Wang, X.; Huang, Y. C.; Shi, Y.; Zhao, X.; Wang, J; Long, R; et al. Angew. Chem. Int. Ed. 2023, 62, e202217369. doi:10.1002/anie.202217369
10. [10]
  (10) Lv, H.; Lv, F.; Qin, H.; Min, X.; Sun, L.; Han, N.; Xu, D.; Li, Y.; Liu, B. CCS Chem. 2022, 4, 1376. doi:10.31635/ccschem.021.202100958
11. [11]
  (11) Li, Z.; He, D.; Yan, X.; Dai, S.; Younan, S.; Ke, Z.; Pan, X.; Xiao, X.; Wu, H.; Gu, J. Angew. Chem. Int. Ed. 2020, 59, 18572. doi:10.1002/anie.202000318
12. [12]
  (12) Guntern, Y. T.; Okatenko, V.; Pankhurst, J.; Varandili, S. B.; Iyengar, P.; Koolen, C.; Stoian, D.; Vavra, J.; Buonsanti, R. ACS Catal. 2021, 11, 1248. doi:10.1021/acscatal.0c04403
13. [13]
  (13) Hammer, B.; Nørskov, J. K. Adv. Catal. 2000, 45, 71. doi:10.1016/S0360-0564(02)45013-4
14. [14]
  (14) Zhang, X.-G.; Jin, X.; Wu, D.-Y.; Tian, Z.-Q. J. Phys. Chem. C. 2018, 122, 25447. doi:10.1021/acs.jpcc.8b08170
15. [15]
  (15) Chang, K.; Jian, X.; Jeong, H. M.; Kwon, Y.; Lu, Q.; Cheng, M. J. J. Phys. Chem. Lett. 2020, 11, 1896. doi:10.1021/acs.jpclett.0c00082
16. [16]
  (16) Xiong, L.; Zhang, X.; Yuan, H.; Wang, J.; Yuan, X.; Lian, Y.; Jin, H.; Sun, H.; Deng, Z.; Wang, D; et al. Angew. Chem. Int. Ed. 2021, 60, 2508. doi:10.1002/anie.202012631
17. [17]
  (17) Choi, C.; Cai, J.; Lee, C.; Lee, H. M.; Xu, M.; Huang, Y. Nano Res. 2021, 14, 3497. doi:10.1007/s12274-021-3639-x
18. [18]
  (18) Ting, L. R. L.; Piqué, O.; Lim, S. Y.; Tanhaei, M.; Calle-Vallejo, F.; Yeo, B. S. ACS Catal. 2020, 10, 4059. doi:10.1021/acscatal.9b05319
19. [19]
  (19) Scarabelli, L.; Sun, M.; Zhuo, X.; Yoo, S.; Millstone, J. E.; Jones, M. R.; Liz-Marzan, L. M. Chem. Rev. 2023, 123, 3493. doi:10.1021/acs.chemrev.3c00033
20. [20]
  (20) Zaza, L.; Rossi, K.; Buonsanti, R. ACS Energy Lett. 2022, 7, 1284. doi:10.1021/acsenergylett.2c00035
21. [21]
  (21) Rong, S.; Wang, X. Chem. Commun. 2022, 58, 11475. doi:10.1039/d2cc04332g
22. [22]
  (22) Xia, Z.; Guo, S. Chem. Soc. Rev. 2019, 48, 3265. doi:10.1039/c8cs00846a
23. [23]
  (23) Yu, S.; Yang, H. Chem. Commun. 2023, 59, 4852. doi:10.1039/d3cc00590a
24. [24]
  (24) Zhang, G.; Ma, Y.; Liu, F.; Tong, Z.; Sha, J.; Zhao, W.; Liu, M.; Zheng, Y. Front. Chem. 2021, 9, 671220. doi:10.3389/fchem.2021.671220
25. [25]
  (25) Segall, M. D.; Lindan, P. J. D.; Probert, M. J.; Pickard, C. J.; Hasnip, P. J.; Clark, S. J.; Payne, M. C. J. Phys.:Condens. Matter 2002, 14, 2717. doi:10.1088/0953-8984/14/11/301
26. [26]
  (26) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865. doi:10.1103/PhysRevLett.77.3865
27. [27]
  (27) Wang, X.; Wang, Z.; García de Arquer, F. P.; Dinh, C.-T.; Ozden, A.; Li, Y. C.; Nam, D.-H.; Li, J.; Liu, Y.-S.; Wicks, J.; et al. Nat. Energy 2020, 5, 478. doi:10.1038/s41560-020-0607-8
28. [28]
  (28) Li, F.; Thevenon, A.; Rosas-Hern;ez, A.; Wang, Z.; Li, Y.; Gabardo, C. M.; Ozden, A.; Dinh, C. T.; Li, J.; Wang, Y.; et al. Nature 2020, 577, 509. doi:10.1038/s41586-019-1782-2
29. [29]
  (29) Wang, Y.; Wang, Z.; Dinh, C.-T.; Li, J.; Ozden, A.; Golam Kibria, M.; Seifitokaldani, A.; Tan, C.-S.; Gabardo, C. M.; Luo,M; et al. Nat. Catal. 2019, 3, 98. doi:10.1038/s41929-019-0397-1
30. [30]
  (30) Govind, N.; Petersen, M.; Fitzgerald, G.; King-Smith, D.; Andzelm, J. Comp. Mater. Sci. 2003, 28, 250. doi:10.1016/s0927-0256(03)00111-3
31. [31]
  (31) Zheng, Y.; Zhang, G.; Ma, Y.; Kong, Y.; Liu, F.; Liu, M. CrystEngComm 2022, 24, 2451. doi:10.1039/D1CE01505B
32. [32]
  (32) Wu, S.; Jia, Q.; Wang, Y.; Liu, F.; Zhang, G.; Zhang, H.; Zhang, H.; Liu, M.; Zheng, Y. Ceram. Int. 2022, 48, 30367. doi:10.1016/j.ceramint.2022.06.310
33. [33]
  (33) Wu, J.; Huang, Y.; Ye, W.; Li, Y. Adv. Sci. 2017, 4, 1700194. doi:10.1002/advs.201700194
34. [34]
  (34) Ou, L.; He, Z.; Yang, H.; Chen, Y. ACS Omega 2021, 6, 17839. doi:10.1021/acsomega.1c01062
35. [35]
  (35) Liu, H.; Yang, B. Chem. Commun. 2022, 58, 709. doi:10.1039/d1cc06735d
36. [36]
  (36) Zhu, C.; Chen, A.; Mao, J.; Wu, G.; Li, S.; Dong, X.; Li, G.; Jiang, Z.; Song, Y. Small. Strut. 2023, 4, 2200328. doi:10.1002/sstr.202200328
37. [37]
  (37) Hammer, B.; Nørskov, J. K. Surf. Sci. 1995, 343, 211. doi:10.1016/0039-6028(96)80007-0
1. [1]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
2. [2]
  Yangrui Xu , Yewei Ren , Xinlin Liu , Hongping Li , Ziyang Lu . 具有高传质和亲和表面的NH₂-UIO-66基疏水多孔液体用于增强CO₂光还原. Acta Physico-Chimica Sinica, 2024, 40(11): 2403032-. doi: 10.3866/PKU.WHXB202403032
3. [3]
  Xuejiao Wang , Suiying Dong , Kezhen Qi , Vadim Popkov , Xianglin Xiang . Photocatalytic CO₂ Reduction by Modified g-C₃N₄. Acta Physico-Chimica Sinica, 2024, 40(12): 2408005-. doi: 10.3866/PKU.WHXB202408005
4. [4]
  Yuejiao An , Wenxuan Liu , Yanfeng Zhang , Jianjun Zhang , Zhansheng Lu . Revealing Photoinduced Charge Transfer Mechanism of SnO₂/BiOBr S-Scheme Heterostructure for CO₂ Photoreduction. Acta Physico-Chimica Sinica, 2024, 40(12): 2407021-. doi: 10.3866/PKU.WHXB202407021
5. [5]
  Yi YANG , Shuang WANG , Wendan WANG , Limiao CHEN . Photocatalytic CO₂ reduction performance of Z-scheme Ag-Cu₂O/BiVO₄ photocatalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 895-906. doi: 10.11862/CJIC.20230434
6. [6]
  Xiutao Xu , Chunfeng Shao , Jinfeng Zhang , Zhongliao Wang , Kai Dai . Rational Design of S-Scheme CeO₂/Bi₂MoO₆ Microsphere Heterojunction for Efficient Photocatalytic CO₂ Reduction. Acta Physico-Chimica Sinica, 2024, 40(10): 2309031-. doi: 10.3866/PKU.WHXB202309031
7. [7]
  Min WANG , Dehua XIN , Yaning SHI , Wenyao ZHU , Yuanqun ZHANG , Wei ZHANG . Construction and full-spectrum catalytic performance of multilevel Ag/Bi/nitrogen vacancy g-C₃N₄/Ti₃C₂T_x Schottky junction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1123-1134. doi: 10.11862/CJIC.20230477
8. [8]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
9. [9]
  Jianyu Qin , Yuejiao An , Yanfeng Zhang . In Situ Assembled ZnWO₄/g-C₃N₄ S-Scheme Heterojunction with Nitrogen Defect for CO₂ Photoreduction. Acta Physico-Chimica Sinica, 2024, 40(12): 2408002-. doi: 10.3866/PKU.WHXB202408002
10. [10]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
11. [11]
  Xiaoling LUO , Pintian ZOU , Xiaoyan WANG , Zheng LIU , Xiangfei KONG , Qun TANG , Sheng WANG . Synthesis, crystal structures, and properties of lanthanide metal-organic frameworks based on 2, 5-dibromoterephthalic acid ligand. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1143-1150. doi: 10.11862/CJIC.20230271
12. [12]
  Ruolin CHENG , Haoran WANG , Jing REN , Yingying MA , Huagen LIANG . Efficient photocatalytic CO₂ cycloaddition over W₁₈O₄₉/NH₂-UiO-66 composite catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 523-532. doi: 10.11862/CJIC.20230349
13. [13]
  Wen YANG , Didi WANG , Ziyi HUANG , Yaping ZHOU , Yanyan FENG . La promoted hydrotalcite derived Ni-based catalysts: In situ preparation and CO₂ methanation performance. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 561-570. doi: 10.11862/CJIC.20230276
14. [14]
  Yongheng Ren , Yang Chen , Hongwei Chen , Lu Zhang , Jiangfeng Yang , Qi Shi , Lin-Bing Sun , Jinping Li , Libo Li . Electrostatically driven kinetic Inverse CO2/C2H2 separation in LTA-type zeolites. Chinese Journal of Structural Chemistry, 2024, 43(10): 100394-100394. doi: 10.1016/j.cjsc.2024.100394
15. [15]
  Qin Cheng , Ming Huang , Qingqing Ye , Bangwei Deng , Fan Dong . Indium-based electrocatalysts for CO₂ reduction to C1 products. Chinese Chemical Letters, 2024, 35(6): 109112-. doi: 10.1016/j.cclet.2023.109112
16. [16]
  Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A. C. Carabineiro , Kangle Lv . Effect of precursors on the structure and photocatalytic performance of g-C3N4 for NO oxidation and CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100416-100416. doi: 10.1016/j.cjsc.2023.100416
17. [17]
  Yi Liu , Zhe-Hao Wang , Guan-Hua Xue , Lin Chen , Li-Hua Yuan , Yi-Wen Li , Da-Gang Yu , Jian-Heng Ye . Photocatalytic dicarboxylation of strained C–C bonds with CO₂ via consecutive visible-light-induced electron transfer. Chinese Chemical Letters, 2024, 35(6): 109138-. doi: 10.1016/j.cclet.2023.109138
18. [18]
  Tong Zhou , Xue Liu , Liang Zhao , Mingtao Qiao , Wanying Lei . Efficient Photocatalytic H₂O₂ Production and Cr(VI) Reduction over a Hierarchical Ti₃C₂/In₄SnS₈ Schottky Junction. Acta Physico-Chimica Sinica, 2024, 40(10): 2309020-. doi: 10.3866/PKU.WHXB202309020
19. [19]
  Muhammad Humayun , Mohamed Bououdina , Abbas Khan , Sajjad Ali , Chundong Wang . Designing single atom catalysts for exceptional electrochemical CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100193-100193. doi: 10.1016/j.cjsc.2023.100193
20. [20]
  Hong Dong , Feng-Ming Zhang . Covalent organic frameworks for artificial photosynthetic diluted CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(7): 100307-100307. doi: 10.1016/j.cjsc.2024.100307

Get Citation

PDF

XML

Metrics

PDF Downloads(1)
Abstract views(389)
HTML views(31)

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

多级钯-铜-银多孔纳米花作为高效电催化剂催化CO2还原为C2+产物

Metrics

通讯作者: 陈斌, bchen63@163.com

多级钯-铜-银多孔纳米花作为高效电催化剂催化CO₂还原为C₂₊产物