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
1. [1]
  Qiaojia GUO , Junkai CAI , Chunying DUAN . Effects of anions on the structural regulation of Zn-salen-modified metal-organic cage. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2203-2211. doi: 10.11862/CJIC.20240209
2. [2]
  Zhengzheng LIU , Pengyun ZHANG , Chengri WANG , Shengli HUANG , Guoyu YANG . Synthesis, structure, and electrochemical properties of a sandwich-type {Co₆}-cluster-added germanotungstate. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1173-1179. doi: 10.11862/CJIC.20240039
3. [3]
  Juan CHEN , Guoyu YANG . A porous-layered aluminoborate built by mixed oxoboron clusters and AlO₄ tetrahedra. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 193-200. doi: 10.11862/CJIC.20240341
4. [4]
  Han ZHANG , Jianfeng SUN , Jinsheng LIANG . Hydrothermal synthesis and luminescent properties of broadband near-infrared Na₃CrF₆ phosphor. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 349-356. doi: 10.11862/CJIC.20240098
5. [5]
  Zhaojun Liu , Zerui Mu , Chuanbo Gao . Alloy nanocrystals: Synthesis paradigms and implications. Chinese Journal of Structural Chemistry, 2023, 42(11): 100156-100156. doi: 10.1016/j.cjsc.2023.100156
6. [6]
  Yinghui Xia , Yixi Lin , Zhenming Xu . Cation potential guiding structural regulation of lithium halide superionic conductors. Chinese Journal of Structural Chemistry, 2025, 44(3): 100448-100448. doi: 10.1016/j.cjsc.2024.100448
7. [7]
  Xian Yan , Huawei Xie , Gao Wu , Fang-Xing Xiao . Boosted solar water oxidation steered by atomically precise alloy nanocluster. Chinese Chemical Letters, 2025, 36(1): 110279-. doi: 10.1016/j.cclet.2024.110279
8. [8]
  Kaili Wang , Pengcheng Liu , Mingzhe Wang , Tianran Wei , Jitao Lu , Xingling Zhao , Zaiyong Jiang , Zhimin Yuan , Xijun Liu , Jia He . Modulating d-d orbitals coupling in PtPdCu medium-entropy alloy aerogels to boost pH-general methanol electrooxidation performance. Chinese Chemical Letters, 2025, 36(4): 110532-. doi: 10.1016/j.cclet.2024.110532
9. [9]
  Yanling Yang , Zhenfa Ding , Huimin Wang , Jianhui Li , Yanping Zheng , Hongquan Guo , Li Zhang , Bing Yang , Qingqing Gu , Haifeng Xiong , Yifei Sun . Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation. Chinese Chemical Letters, 2024, 35(4): 108585-. doi: 10.1016/j.cclet.2023.108585
10. [10]
  Xiaoxue Li , Hongwei Zhou , Rongrong Qian , Xu Zhang , Lei Yu . A concise synthesis of Se/Fe materials for catalytic oxidation reactions of anthracene and polyene. Chinese Chemical Letters, 2025, 36(3): 110036-. doi: 10.1016/j.cclet.2024.110036
11. [11]
  Yu-Yao Li , Xiao-Hui Li , Zhi-Xuan An , Yang Chu , Xiu-Li Wang . Room-temperature olefin epoxidation reaction by two 2D cobalt metal-organic complexes under O₂ atmosphere: Coordination and structural regulation. Chinese Chemical Letters, 2025, 36(4): 109716-. doi: 10.1016/j.cclet.2024.109716
12. [12]
  Shuaiwen Li , Zihui Chen , Feng Yang , Wanqing Yue . The age of vanadium-based nanozymes: Synthesis, catalytic mechanisms, regulation and biomedical applications. Chinese Chemical Letters, 2024, 35(4): 108793-. doi: 10.1016/j.cclet.2023.108793
13. [13]
  Bohan Zhang , Bingzhe Wang , Guichuan Xing , Zikang Tang , Songnan Qu . Regulation of the multi-emission centers in carbon dots via a bottom-up synthesis approach. Chinese Chemical Letters, 2024, 35(9): 109358-. doi: 10.1016/j.cclet.2023.109358
14. [14]
  Shengfei Dong , Ziyu Liu , Xiaoyi Yang . Hydrothermal liquefaction of biomass for jet fuel precursors: A review. Chinese Chemical Letters, 2024, 35(8): 109142-. doi: 10.1016/j.cclet.2023.109142
15. [15]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
16. [16]
  Yiwen Lin , Yijie Chen , Chunhui Deng , Nianrong Sun . Integration of resol/block-copolymer carbonization and machine learning: A convenient approach for precise monitoring of glycan-associated disorders. Chinese Chemical Letters, 2024, 35(12): 109813-. doi: 10.1016/j.cclet.2024.109813
17. [17]
  Changlin Su , Wensheng Cai , Xueguang Shao . Water as a probe for the temperature-induced self-assembly transition of an amphiphilic copolymer. Chinese Chemical Letters, 2025, 36(4): 110095-. doi: 10.1016/j.cclet.2024.110095
18. [18]
  Pingfan Zhang , Shihuan Hong , Ning Song , Zhonghui Han , Fei Ge , Gang Dai , Hongjun Dong , Chunmei Li . Alloy as advanced catalysts for electrocatalysis: From materials design to applications. Chinese Chemical Letters, 2024, 35(6): 109073-. doi: 10.1016/j.cclet.2023.109073
19. [19]
  Qian Wang , Ting Gao , Xiwen Lu , Hangchao Wang , Minggui Xu , Longtao Ren , Zheng Chang , Wen Liu . Nanophase separated, grafted alternate copolymer styrene-maleic anhydride as an efficient room temperature solid state lithium ion conductor. Chinese Chemical Letters, 2024, 35(7): 108887-. doi: 10.1016/j.cclet.2023.108887
20. [20]
  Chunru Liu , Ligang Feng . Advances in anode catalysts of methanol-assisted water-splitting reactions for hydrogen generation. Chinese Journal of Structural Chemistry, 2023, 42(10): 100136-100136. doi: 10.1016/j.cjsc.2023.100136

Get Citation

PDF

XML

Metrics

PDF Downloads(2)
Abstract views(984)
HTML views(27)

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