Pt@Au/Al2O3核壳纳米粒子的制备和表征及其在催化氧化甲苯中的应用

doi:10.3866/PKU.WHXB201907057

Abstract

Abstract:

Customizing core-shell nanostructures is considered to be an efficient approach to improve the catalytic activity of metal nanoparticles. Various physiochemical and green methods have been developed for the synthesis of core-shell structures. In this study, a novel liquid-phase hydrogen reduction method was employed to form core-shell Pt@Au nanoparticles with intimate contact between the Pt and Au particles, without the use of any protective or structure-directing agents. The Pt@Au core-shell nanoparticles were prepared by depositing Au metal onto the Pt core; AuCl⁴⁻ was reduced to Au(0) by H₂ in the presence of Pt nanoparticles. The obtained Pt@Au core-shell structured nanoparticles were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), high-resolution TEM, fast Fourier transform, powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and H₂-temperature programmed reduction (H₂-TPR) analyses. The EDX mapping results for the nanoparticles, as obtained from their scanning transmission electron microscopy images in the high-angle annular dark-ﬁeld mode, revealed a Pt core with Au particles grown on its surface. Fourier transform measurements were carried out on the high-resolution structure to characterize the Pt@Au nanoparticles. The lattice plane at the center of the nanoparticles corresponded to Pt, while the edge of the particles corresponded to Au. With an increase in the Au content, the intensity of the peak corresponding to Pt in the FTIR spectrum decreased slowly, indicating that the Pt nanoparticles were surrounded by Au nanoparticles, and thus confirming the core-shell structure of the nanoparticles. The XRD results showed that the peak corresponding to Pt shifted gradually toward the Au peak with an increase in the Au content, indicating that the Au particles grew on the Pt seeds; this trend was consistent with the FTIR results. Hence, it can be stated that the Pt@Au core-shell structure was successfully prepared using the liquid-phase hydrogen reduction method. The catalytic activity of the nanoparticles for the oxidation of toluene was evaluated using a fixed-bed reactor under atmospheric pressure. The XPS and H₂-TPR results showed that the Pt₁@Au₁/Al₂O₃ catalyst had the best toluene oxidation activity owing to its lowest reduction temperature, lowest Au 4d & 4f and Pt 4d & 4f binding energies, and highest Au⁰/Au^δ⁺ and Pt⁰/Pt²⁺ proportions. The Pt₁@Au₂Al₂O₃ catalyst showed high stability under dry and humid conditions. The good catalytic performance and high selectivity of Pt@Au/Al₂O₃ for toluene oxidation could be attributed to the high concentration of adsorbed oxygen species, good low-temperature reducibility, and strong interaction.

Key words: Catalyst, Synergy, Nanomaterials, Core-shell structure, VOCs

Chao Zhang, Sihan Li, Chenliang Wu, Xiaoqing Li, Xinhuan Yan. Preparation and Characterization of Pt@Au/Al₂O₃ Core-Shell Nanoparticles for Toluene Oxidation Reaction[J].Acta Physico-Chimica Sinica, 2020, 36(8): 1907057.

Figures/Tables 10

References 47

1	Zhang Q. ; Lee I. ; Joo J. B. ; Zaera F. ; Yin Y. Acc. Chem. Res. 2012, 46, 1816. doi: 10.1021/ar300230s
2	Sun Q. ; Zhang X. Q. ; Wang Y. ; Lu A. H. Chin. J. Catal. 2015, 36, 683. doi: 10.1016/S1872-2067(14)60298-9
3	Lee J. ; Yoo J. K. ; Kim J. ; Sohn Y. ; Rhee C. K. Electrochim. Acta 2018, 290, 244. doi: 10.1016/j.electacta.2018.09.078
4	Shim K. ; Lee W. C. ; Park M. S. ; Shahabuddin M. ; Yamauchi Y. ; Hossain M. S. A. ; Shim Y. B. ; Kim J. H. Sens. Actuator B-Chem. 2019, 278, 88. doi: 10.1016/j.snb.2018.09.048
5	Zhou S. ; McIlwrath K. ; Jackson G. ; Eichhorn B. J. Am. Chem. Soc. 2006, 128, 1780. doi: 10.1021/ja056924
6	Jiang R. ; Tung S. O. ; Tang Z. ; Li L. ; Ding L. ; Xi X. ; Liu Y. ; Zhang L. ; Zhang J. Energy Storage Mater. 2018, 12, 260. doi: 10.1016/j.ensm.2017.11.005
7	Jiang L. ; Yuan X. ; Liang J. ; Zhang J. ; Wang H. ; Zeng G. J. Power Sources 2016, 331, 408. doi: 10.1016/j.jpowsour.2016.09.054
8	Campani V. ; Giarra S. ; De Rosa G. OpenNano 2018, 3, 5. doi: 10.1016/j.onano.2017.12.001
9	Chen G. ; Wang Y. ; Xie R. ; Gong S. Adv. Drug Delivery Rev. 2018, 130, 58. doi: 10.1016/j.addr.2018.07.008
10	Zhang N. ; Liu S. ; Xu Y. Nanoscale 2012, 4, 2227. doi: 10.1039/c2nr00009a
11	Tada H. ; Suzuki F. ; Ito S. ; Akita T. ; Tanaka K. ; Kawahara T. ; Kobayashi H. J. Phys. Chem. B 2002, 106, 8714. doi: 10.1021/jp0202690
12	Yoon J. ; Baik H. ; Lee S. ; Kwon S. J. ; Lee K. Nanoscale 2014, 6, 6434. doi: 10.1039/c4nr00551a
13	Yang C. ; Zhang F. ; Lei N. ; Yang M. ; Liu F. ; Miao Z. ; Sun Y. ; Zhao X. ; Wang A. Chin. J. Catal. 2018, 39, 1366. doi: 10.1016/s1872-2067(18)63103-1
14	Zhang Y. ; Liu Y. ; Xie S. ; Huang H. ; Guo G. ; Dai H. ; Deng J. Environ. Int. 2019, 128, 335. doi: 10.1016/j.envint.2019.04.062
15	Qi Y. ; Shen L. ; Zhang J. ; Yao J. ; Lu R. ; Miyakoshi T. Environ. Pollut. 2019, 245, 810. doi: 10.1016/j.envpol.2018.11.057
16	Morin J. ; Gandolfo A. ; Temime-Roussel B. ; Strekowski R. ; Brochard G. ; Bergé. V% Gligorovski S. ; Wortham H. Build. Environ. 2019, 156, 225. doi: 10.1016/j.buildenv.2019.04.031
17	Song M. ; Liu X. ; Zhang Y. ; Shao M. ; Lu K. ; Tan Q. ; Feng M. ; Qu Y. Atmos. Environ. 2019, 201, 28. doi: 10.1016/j.atmosenv.2018.12.019
18	Kim K. ; Boo S. ; Ahn H. J. Ind. Eng. Chem. 2009, 15, 92. doi: 10.1016/j.jiec.2008.09.005
19	Zhu A. ; Zhou Y. ; Wang Y. ; Zhu Q. ; Liu H. ; Zhang Z. ; Lu H. J. Rare Earths 2018, 36, 1272. doi: 10.1016/j.jre.2018.03.032
20	Feng Z. ; Ma Y. ; Natarajan V. ; Zhao Q. ; Ma X. ; Zhan J. Sens. Actuator B-Chem. 2018, 255, 884. doi: 10.1016/j.snb.2017.08.138
21	Gaálová J. ; Topka P. ; Kaluža L. ; Soukup K. ; Barbier J. Catal. Today. 2019, 333, 190. doi: 10.1016/j.cattod.2018.04.005
22	Vallejos S. ; Gràcia I. ; Bravo J. ; Figueras E. ; Hubálek J. ; Cané C. Talanta 2015, 139, 27. doi: 10.1016/j.talanta.2015.02.034
23	Usón L. ; Colmenares M. G. ; Hueso J. L. ; Sebastián V. ; Balas F. ; Arruebo M. ; Santamaría J. Catal. Today 2014, 227, 179. doi: 10.1016/j.cattod.2013.08.014
24	Mori M. ; Nishimura H. ; Itagaki Y. ; Sadaoka Y. ; Traversa E. Sens. Actuator B-Chem. 2009, 143, 56. doi: 10.1016/j.snb.2009.09.001
25	Li J. H. ; Ao P. ; Li X. Q. ; Xu X. S. ; Xu X. X. ; Gao X. ; Yan X. H. Acta Phys. -Chim. Sin. 2015, 31, 173. doi: 10.3866/PKU.WHXB201411131
	李加衡; 敖平; 李小青; 许响生; 徐潇潇; 高翔; 严新焕. 物理化学学报, 2015, 31, 173. doi: 10.3866/PKU.WHXB201411131
26	Sun S. ; Wang Y. ; Wang L. N. ; Guo T. ; Yuan X. ; Zhang D. ; Xue Z. ; Zhou X. ; Lu X. J. Alloy. Compd. 2019, 793, 635. doi: 10.1016/j.jallcom.2019.04.212
27	Peng C. ; Pan N. ; Qian Z. ; Wei X. ; Shao G. Talanta 2017, 175, 114. doi: 10.1016/j.talanta.2017.06.005
28	Takahashi S. ; Todoroki N. ; Myochi R. ; Nagao T. ; Taguchi N. ; Ioroi T. ; Feiten F. E. ; Wakisaka Y. ; Asakura K. ; Sekizawa O. ; et al J. Electroanal. Chem. 2019, 842, 1. doi: 10.1016/j.jelechem.2019.04.053
29	Lewis L. N. ; Krafft T. A. ; Huffman J. C. Inorg. Chem. 1992, 31, 3555. doi: 10.1021/ic00043a014
30	Kristian N. ; Wang X. Electrochem. Commun. 2008, 10, 12. doi: 10.1016/j.elecom.2007.10.011
31	Grzelczak M. ; Pérez-Juste J. ; Rodríguez-González B. ; Liz-Marzán L. M. J. Mater. Chem. 2006, 16, 3946. doi: 10.1039/b606887a
32	Liao M. ; Li W. ; Xi X. ; Luo C. ; Gui S. ; Jiang C. ; Mai Z. ; Chen B. H. J. Electroanal. Chem. 2017, 791, 124. doi: 10.1016/j.jelechem.2017.03.024
33	Cao R. ; Xia T. ; Zhu R. ; Liu Z. ; Guo J. ; Chang G. ; Zhang Z. ; Liu X. ; He Y. Appl. Surf. Sci. 2018, 433, 840. doi: 10.1016/j.apsusc.2017.10.104
34	Nishita M. ; Park S. Y. ; Nishio T. ; Kamizaki K. ; Wang Z. ; Tamada K. ; Takumi T. ; Hashimoto R. ; Otani H. ; Pazour G. J. ; et al Sci. Rep. 2017, 7, 1306. doi: 10.1038/s41598-016-0028-x
35	Guo S. ; Li J. ; Dong S. ; Wang E. J. Phys. Chem. C 2010, 114, 15337. doi: 10.1021/jp104942d
36	Yang H. ; Deng J. ; Liu Y. ; Xie S. ; Wu Z. ; Dai H. J. Mol. Catal. A-Chem. 2016, 414, 9. doi: 10.1016/j.molcata.2015.12.010
37	Pei W. ; Liu Y. ; Deng J. ; Zhang K. ; Hou Z. ; Zhao X. ; Dai H. Appl. Catal. B-Environ. 2019, 256, 117814. doi: 10.1016/j.apcatb.2019.117814
38	He G. ; Song Y. ; Liu K. ; Walter A. ; Chen S. ; Chen S. ACS Catal. 2013, 3, 831. doi: 10.1021/cs400114s
39	Zhang X. ; Li Z. ; Zhao J. ; Cui Y. ; Tan B. ; Wang J. ; Zhang C. ; He G. Korean J. Chem. Eng. 2017, 34, 1. doi: 10.1007/s11814-017-0092-3
40	Lefèvre G. ; Duc M. ; Lepeut P. ; Caplain R. ; Fédoroff M. Langmuir 2002, 18, 7530. doi: 10.1021/la025651i
41	Meng T. ; Wang L. ; Jia H. ; Gong T. ; Feng Y. ; Li R. ; Wang H. ; Zhang Y. J. Colloid Interface Sci. 2019, 536, 424. doi: 10.1016/j.jcis.2018.10.076
42	Cao Z. ; Bu J. ; Zhong Z. ; Sun C. ; Zhang Q. ; Wang J. ; Chen S. ; Xie X. Appl. Catal. A-Gen. 2019, 578, 105. doi: 10.1016/j.apcata.2019.04.006
43	Chenakin S. ; Kruse N. J. Catal. 2018, 358, 224. doi: 10.1016/j.jcat.2017.12.010
44	Figueiredo N. M. ; Carvalho N. J. M. ; Cavaleiro A. Appl. Surf. Sci. 2011, 257, 5793. doi: 10.1016/j.apsusc.2011.01.104
45	Nartova A. V. ; Gharachorlou A. ; Bukhtiyarov A. V. ; Kvon R. I. ; Bukhtiyarov V. I. Appl. Surf. Sci. 2017, 401, 341. doi: 10.1016/j.apsusc.2016.12.179
46	Smirnov M. Y. ; Kalinkin A. V. ; Vovk E. I. ; Simonov P. A. ; Gerasimov E. Y. ; Sorokin A. M. ; Bukhtiyarov V. I. Appl. Surf. Sci. 2018, 428, 972. doi: 10.1016/j.apsusc.2017.09.205
47	Ousmane M. ; Liotta L. F. ; Carlo G. D. ; Pantaleo G. ; Venezia A. M. ; Deganello G. ; Retailleau L. ; Boreave A. ; Giroir-Fendler A. Appl. Catal. B-Environ. 2011, 101, 629. doi: 10.1016/j.apcatb.2010.11.004

[1]	Yaowu Luo, Dingsheng Wang. Enhancing Heterogeneous Catalysis by Electronic Property Regulation of Single Atom Catalysts [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212020-0.
[2]	Weifeng Xia, Chengyu Ji, Rui Wang, Shilun Qiu, Qianrong Fang. Metal-Free Tetrathiafulvalene Based Covalent Organic Framework for Efficient Oxygen Evolution Reaction [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212057-0.
[3]	Zhanjun He, Min Huang, Tiejun Lin, Liangshu Zhong. Recent Advances in Dry Reforming of Methane via Photothermocatalysis [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212060-0.
[4]	Qianwei Song, Guanchao He, Huilong Fei. Photothermal Catalytic Conversion Based on Single Atom Catalysts: Fundamentals and Applications [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212038-0.
[5]	Yucui Hou, Zhuosen He, Shuhang Ren, Weize Wu. Catalytic Oxidation of Biomass to Formic Acid under O₂ with Homogeneous Catalysts [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212065-0.
[6]	Meng Li, Fulin Yang, Jinfa Chang, Alex Schechter, Ligang Feng. MoP-NC Nanosphere Supported Pt Nanoparticles for Efficient Methanol Electrolysis [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2301005-0.
[7]	Yanhui Yu, Peng Rao, Suyang Feng, Min Chen, Peilin Deng, Jing Li, Zhengpei Miao, Zhenye Kang, Yijun Shen, Xinlong Tian. Atomic Co Clusters for Efficient Oxygen Reduction Reaction [J]. Acta Phys. -Chim. Sin., 2023, 39(8): 2210039-0.
[8]	Chang Lan, Yuyi Chu, Shuo Wang, Changpeng Liu, Junjie Ge, Wei Xing. Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts [J]. Acta Phys. -Chim. Sin., 2023, 39(8): 2210036-0.
[9]	Shanshan Shen, Xiaohui Liu, Yong Guo, Yanqin Wang. Performance Enhancement of Pt/Silicalite-1 by in situ Doped Fe for Propane Dehydrogenation [J]. Acta Phys. -Chim. Sin., 2023, 39(7): 2209043-0.
[10]	. Giant Enhancement of Optical Second Harmonic Generation in Hollow-Core Fiber Integrated with GaSe Nanoflakes [J]. Acta Phys. -Chim. Sin., 2023, 39(7): 2212028-0.
[11]	. S-Scheme Heterojunction of Cu₂O Polytope-Modified BiOI Sheet for Efficient Visible-Light-Driven CO₂ Conversion under Water Vapor [J]. Acta Phys. -Chim. Sin., 2023, 39(6): 2210003-0.
[12]	Jingjing Wang, Guiqiang Cao, Ruixian Duan, Xiangyang Li, Xifei Li. Advances in Single Metal Atom Catalysts Enhancing Kinetics of Sulfur Cathode [J]. Acta Phys. -Chim. Sin., 2023, 39(5): 2212005-0.
[13]	Yanke Yu, Mengqiao Geng, Desheng Wei, Chi He. Effect of Potassium on the Performance of a CuSO₄/TiO₂ Catalyst Used in the Selective Catalytic Reduction of NO_x by NH₃ [J]. Acta Phys. -Chim. Sin., 2023, 39(4): 2206034-0.
[14]	Tianmi Tang, Zhenlu Wang, Jingqi Guan. Electronic Structure Regulation of Single-Site M-N-C Electrocatalysts for Carbon Dioxide Reduction [J]. Acta Phys. -Chim. Sin., 2023, 39(4): 2208033-0.
[15]	Erjun Lu, Junqian Tao, Can Yang, Yidong Hou, Jinshui Zhang, Xinchen Wang, Xianzhi Fu. Carbon-Encapsulated Pd/TiO₂ for Photocatalytic H₂ Evolution Integrated with Photodehydrogenative Coupling of Amines to Imines [J]. Acta Phys. -Chim. Sin., 2023, 39(4): 2211029-0.

Preparation and Characterization of Pt@Au/Al₂O₃ Core-Shell Nanoparticles for Toluene Oxidation Reaction

RichHTML

PDF

Like

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 10

References 47

Related Articles 15

Metrics

Recommended 0

Preparation and Characterization of Pt@Au/Al2O3 Core-Shell Nanoparticles for Toluene Oxidation Reaction

RichHTML

PDF

Like

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 10

References 47

Related Articles 15

Metrics

Recommended 0

Preparation and Characterization of Pt@Au/Al₂O₃ Core-Shell Nanoparticles for Toluene Oxidation Reaction