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

MSC2000:

O643

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]	Xuemei Zhou. TiO₂-Supported Single-Atom Catalysts for Photocatalytic Reactions [J]. Acta Phys. -Chim. Sin., 2021, 37(6): 2008064-0.
[2]	Yichen Meng, Siyu Kuang, Hai Liu, Qun Fan, Xinbin Ma, Sheng Zhang. Recent Advances in Electrochemical CO₂ Reduction Using Copper-Based Catalysts [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2006034-0.
[3]	Xinjiang Cui, Feng Shi. Selective Conversion of CO₂ by Single-Site Catalysts [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2006080-0.
[4]	Jin Wu, Jing Liu, Wu Xia, Ying-Yi Ren, Feng Wang. Advances on Photocatalytic CO₂ Reduction Based on CdS and CdSe Nano-Semiconductors [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2008043-0.
[5]	Yanqiu Wang, Zixin Zhong, Tangkang Liu, Guoliang Liu, Xinlin Hong. Cu@UiO-66 Derived Cu⁺-ZrO₂ Interfacial Sites for Efficient CO₂ Hydrogenation to Methanol [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2007089-0.
[6]	Congming Li, Kuo Chen, Xiaoyue Wang, Nan Xue, Hengquan Yang. Understanding the Role of Cu/ZnO Interaction in CO₂ Hydrogenation to Methanol [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2009101-0.
[7]	Lin Li, Shuiyun Shen, Guanghua Wei, Junliang Zhang. Electrocatalytic Activity of Hemin-Derived Hollow Non-Precious Metal Catalyst for Oxygen Reduction Reaction [J]. Acta Phys. -Chim. Sin., 2021, 37(3): 1911011-0.
[8]	Yuan Zhou, Na Han, Yanguang Li. Recent Progress on Pd-based Nanomaterials for Electrochemical CO₂ Reduction [J]. Acta Physico-Chimica Sinica, 2020, 36(9): 2001041-0.
[9]	Jian Zhang, Liang Wang, Zhiyi Wu, Chengtao Wang, Zerui Su, Feng-Shou Xiao. Rational Design of a Core-Shell Rh@Zeolite Catalyst for Selective Diene Hydrogenation [J]. Acta Phys. -Chim. Sin., 2020, 36(9): 1912001-0.
[10]	Yimeng Wang, Shenping Zhang, Yu Ge, Chenhui Wang, Jun Hu, Honglai Liu. Highly Efficient Photocatalytic Degradation of Tetracycline Using a Bimetallic Oxide/Carbon Photocatalyst [J]. Acta Physico-Chimica Sinica, 2020, 36(8): 1905083-0.
[11]	Danye Liu,Dong Chen,Hui Liu,Jun Yang. Inside-Out Migration of Noble Metals in Ag₂S Nanoparticles [J]. Acta Physico-Chimica Sinica, 2020, 36(7): 1906069-0.
[12]	Dongmei Liu,Xiumei Chen,Ze Yuan,Min Lu,Lisha Yin,Xiaoji Xie,Ling Huang. Coating and Transforming the Y(OH)CO₃ Shell on Upconversion Nanoparticles [J]. Acta Physico-Chimica Sinica, 2020, 36(7): 1907011-0.
[13]	Bo Fang,Ligang Feng. PtCo-NC Catalyst Derived from the Pyrolysis of Pt-Incorporated ZIF-67 for Alcohols Fuel Electrooxidation [J]. Acta Physico-Chimica Sinica, 2020, 36(7): 1905023-0.
[14]	Liang Wang,Chenglu Zhu,Lisha Yin,Wei Huang. Construction of Pt-M (M = Co, Ni, Fe)/g-C₃N₄ Composites for Highly Efficient Photocatalytic H₂ Generation [J]. Acta Physico-Chimica Sinica, 2020, 36(7): 1907001-0.
[15]	Jing Miao,Ruifeng Guo,Zhihong Liu. Preparation of BaO·4B₂O₃·5H₂O Nanomaterial and Evaluation of Its Flame Retardant Performance to PP by Thermal Decomposition Kinetics Method [J]. Acta Physico-Chimica Sinica, 2020, 36(6): 1905052-0.

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

Comments

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

Comments

Recommended 0

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