Citation: Xinwen ZHOU, Xiaoyu SHEN, Ce FU, Pan WANG, Luoyi YAN, Zheng CHENG, Guixian TIAN, Ronghua ZHANG. Effects of synthesis and structural regulation of Ir and IrPd catalysts on methanol oxidation performance[J]. Chinese Journal of Inorganic Chemistry, ;2024, 40(2): 412-420. doi: 10.11862/CJIC.20230288 shu

Effects of synthesis and structural regulation of Ir and IrPd catalysts on methanol oxidation performance

Xinwen ZHOU ^{1, 2,,} ,
Xiaoyu SHEN ¹ ,
Ce FU ¹ ,
Pan WANG ¹ ,
Luoyi YAN ¹ ,
Zheng CHENG ¹ ,
Guixian TIAN ¹ ,
Ronghua ZHANG ^{1, 2,,}

1.
College of Materials and Chemical Engineering, China Three Gorges University, Yichang, Hubei 443002, China
2.
Hubei Three Gorges Laboratory, Yichang, Hubei 443002, China

Corresponding author: Xinwen ZHOU, xwzhou@ctgu.edu.cn Ronghua ZHANG, rhzhang@ctgu.edu.cn
Received Date: 2 August 2023
Revised Date: 5 December 2023

Figures(6)

Using triblock copolymer P123 (poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide), PEO₂₀-PPO₇₀-PEO₂₀) as reducing agent and protective agent, the effects of hydrothermal and solvothermal methods on the synthesis of pure Ir and IrPd alloy catalysts and their electrocatalytic oxidation of methanol (MOR) were compared. For pure Ir catalyst, solvothermal method can better promote the reduction of Ir precursor under the same condi- tions. For IrPd alloy catalysts, core-shell structure products (IrPd-S) with rich Ir-surface but low MOR activity can be prepared by solvothermal method. The different atomic ratios (IrPd, Ir2Pd, IrPd2) obtained by hydrothermal reaction have smaller particle sizes and more uniform distribution of elements. Among them, IrPd catalyst with ratio of 1∶1 (IrPd-H) had the highest MOR electrocatalytic activity. These results show that the structure, surface composition and electrocatalytic activity of pure Ir and IrPd alloy catalysts can be effectively adjusted by adjusting the type of solvent and the structural induction of P123.
- structural regulation,
- hydrothermal synthesis,
- IrPd alloy,
- triblock copolymer,
- oxidation of methanol
1. [1]
  Quinson J. Iridium and IrO_x nanoparticles: An overview and review of syntheses and applications[J]. Adv. Colloid Interface Sci., 2022,303102643. doi: 10.1016/j.cis.2022.102643
2. [2]
  ZHUANG Z H, CHEN W. Application of atomically precise metal nanoclusters in electrocatalysis[J]. J. Electrochem., 2021,27(2):125-143.
3. [3]
  Wang S, Shen T, Yang C, Luo G Y, Wang D L. Engineering iridium-based oxygen evolution reaction electrocatalysts for proton exchange membrane water electrolyzers[J]. ACS Catal., 2023,13(13):8670-8691. doi: 10.1021/acscatal.3c01511
4. [4]
  Liu Y P, Liang X, Chen H, Gao R Q, Shi L, Yang L, Zou X X. Iridium-containing water-oxidation catalysts in acidic electrolyte[J]. Chin. J. Catal., 2021,42(7):1054-1077. doi: 10.1016/S1872-2067(20)63722-6
5. [5]
  HU P J, WU Y N, ZHENG H Y, MENG L, JIN L Y, LUO M F. Ir/CeO₂ catalysts: Characterization and performance for CO oxidation[J]. Chinese J. Inorg. Chem., 2011,27(12):2389-2394.
6. [6]
  Quinson J, Kacenauskaite L, Schröder J, Simonsen S B, Kuhn L T, Vosch T, Arenz M. UV-induced syntheses of surfactant-free precious metal nanoparticles in alkaline methanol and ethanol[J]. Nanoscale Adv., 2020,2:2288-2292. doi: 10.1039/D0NA00218F
7. [7]
  Cooper C, Dooley K M, Fierro-Gonzalez J C, Guzman J, Jentoft R, Lamb H H, Ogino L, Runnebaum R C, Sapre A, Uzun A. Bruce gates: A career in catalysis[J]. ACS Catal., 2020,10:11912-11935. doi: 10.1021/acscatal.0c03568
8. [8]
  Jin G X, Liu J, Wang C, Gu W X, Ran G X, Liu B, Song Q J. Ir nanoparticles with multi-enzyme activities and its application in the selective oxidation of aromatic alcohols[J]. Appl. Catal. B-Environ., 2020,267(15)118725.
9. [9]
  Zhu J Y, Xue Q, Xue Y Y, Ding Y, Li F M, Jin P, Chen P, Chen Y. Iridium nanotubes as bifunctional electrocatalysts for oxygen evolution and nitrate reduction reactions[J]. ACS Appl. Mater. Interfaces, 2020,12:14064-14070. doi: 10.1021/acsami.0c01937
10. [10]
  Cai C, Wang M Y, Han S B, Wang Q, Zhang Q, Zhu Y M, Yang X M, Wu D J, Zu X T, Sterbinkey G E, Feng Z X, Gu M. Ultrahigh oxygen evolution reaction activity achieved using Ir single atoms on amorphous CoO_x nanosheets[J]. ACS Catal., 2020,11:123-130.
11. [11]
  Zhou X W, Gan Y L, Dai Z X, Zhang R H. Monodispersed Pd nanospheres and their electrocatalytic properties for methanol oxidation in alkaline medium[J]. J. Electroanal. Chem., 2012,685:97-102. doi: 10.1016/j.jelechem.2012.08.036
12. [12]
  Yang Y, Du J J, Luo L M, Zhang R H, Dai Z X, Zhou X W. Facile aqueous-phase synthesis and electrochemical properties of novel PtPd hollow nanocatalysts[J]. Electrochim. Acta, 2016,212:966-972. doi: 10.1016/j.electacta.2016.07.085
13. [13]
  Yang Y, Luo L M, Guo Y F, Dai Z X, Zhang R H, Sun C, Zhou X W. In situ synthesis of PtPd bimetallic nanocatalysts supported on graphene nanosheets for methanol oxidation using triblock copolymer as reducer and stabilizer[J]. J. Electroanal. Chem., 2016,783:132-139. doi: 10.1016/j.jelechem.2016.11.034
14. [14]
  Luo L M, Zhang R H, Du J J, Yang F, Liu H M, Yang Y, Zhou X W. Studies on the synthesis and electrocatalytic properties of hollow PdAu nanocatalysts[J]. Int. J. Hydrog. Energy, 2017,42:16139-16148. doi: 10.1016/j.ijhydene.2017.03.015
15. [15]
  Hu Q Y, Zhan W, Guo Y F, Luo L M, Zhang R H, Chen D, Zhou X W. Heat treatment bimetallic PdAu nanocatalyst for oxygen reduction reaction[J]. J. Energy Chem., 2020,40:217-223. doi: 10.1016/j.jechem.2019.05.011
16. [16]
  Fu C, Wang P, Zhang R H, Yan L Y, Cheng Z, Zhang X, Zhou X W. Efficient synthesis of PdIr nanocatalysts with controllable surface composition for electrochemical oxidation of methanol[J]. Fuel, 2023,332126105. doi: 10.1016/j.fuel.2022.126105
17. [17]
  Xu Z H, Yin Q C, Li X, Meng Q, Xu L S, Lv B S, Zhang G L. Self- assembly of a highly stable and active Co₃O₄/H-TiO₂ bulk heterojunction with high-energy interfacial structures for low temperature CO catalytic oxidation[J]. Catal. Sci. Technol., 2020,10(24):8374-8382. doi: 10.1039/D0CY01477J
18. [18]
  Kundu S, Liang H. Shape-selective formation and characterization of catalytically active iridium nanoparticles[J]. J. Colloid Interface Sci., 2011,354:597-606. doi: 10.1016/j.jcis.2010.11.032
19. [19]
  YANG Y, LUO L M, DU J J, ZHANG R H, DAI Z X, ZHOU X W. Hollow Pt-based nanocatalysts synthesized through galvanic replacement reaction applied in proton exchange membrane fuel cells[J]. Acta Phys.-Chim. Sin., 2016,32(4):834-847.
20. [20]
  Hu Q Y, Zhang R H, Chen D, Guo Y F, Zhan W, Luo L M, Zhou X W. Facile aqueous phase synthesis of 3D-netlike PdRh nanocatalysts for methanol oxidation[J]. Int. J. Hydrog. Energy, 2019,44:16287-16296. doi: 10.1016/j.ijhydene.2019.05.048
21. [21]
  Zhan W, Cheng Z, Zhang R H, Yan L Y, Tian G X, Lin D H, Xiao S Z, Zhou X W. In situ construction of chain-like PdAg/AgCl heterojunction electrocatalyst for ethylene glycol oxidation[J]. J. Electroanal. Chem., 2023,942117547. doi: 10.1016/j.jelechem.2023.117547
22. [22]
  Lee Y W, Kim M J, Kim Z H, Ham S W. One-step synthesis of Au@Pd core-shell nanooctahedron[J]. J. Am. Chem. Soc., 2009,131:17036-17037. doi: 10.1021/ja905603p
23. [23]
  Guo K, Fan D P, Teng Y X, Xu D D, Li Y F, Bao J C. Engineering PdIr nanostructures synergistically induced by self-assembled surfactants and halide ions for alcohol electrooxidation[J]. Chem.-Eur. J., 2022,28e202200053. doi: 10.1002/chem.202200053
24. [24]
  Shi J Y, Kao C W, Lan J, Jiang K, Peng M, Luo M, Lu Y R, Zhang S G, Tan Y W. Nanoporous PdIr alloy for high-efficiency and durable water splitting in acidic media[J]. J. Mater. Chem. A, 2023,11:11526-11533. doi: 10.1039/D3TA01280H
25. [25]
  Pulm H, Hohlneicher G, Freund H J, Schushter H U, Drews J, Eberv U. Charge distribution in some ternary vintl phases as studied by v-ray photoelectron spectroscopy[J]. J. Less-Common. Met., 1986,115:127-143. doi: 10.1016/0022-5088(86)90378-4
26. [26]
  Dückers K, Bonzel H P. Core and valence level spectroscopy with Y Mζ radiation: CO and K on (110) surfaces of Ir, Pt and Au[J]. Surf. Sci., 1989,213:25-48. doi: 10.1016/0039-6028(89)90251-3
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