热处理温度对Pt/TiO<sub>2</sub>纳米带复合物催化HCHO氧化性能的影响

崔维怡; 王希越; 谭乃迪

doi:10.1016/S1872-5813(21)60113-5

热处理温度对Pt/TiO₂纳米带复合物催化HCHO氧化性能的影响

doi: 10.1016/S1872-5813(21)60113-5

崔维怡^{1, 2,},
王希越²,
谭乃迪^2, ,

1.
吉林化工学院化工清洁生产技术吉林省高校重点实验室，吉林吉林 132022
2.
吉林化工学院化学与制药工程学院，吉林吉林 132022

基金项目: 国家自然科学基金（51805207），吉林省教育厅2021科学技术研究规划项目（JJKH20210235KJ）资助

详细信息

作者简介:
崔维怡：cuiweiyi0119@163.com

通讯作者:
E-mail: tannd0119@163.com

中图分类号: TQ426
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- 文章访问数: 330
- HTML全文浏览量: 65
- PDF下载量: 18
- 被引次数: 0
出版历程
- 收稿日期: 2021-03-26
- 修回日期: 2021-05-06
- 网络出版日期: 2021-06-12
- 刊出日期: 2021-11-30

Effect of thermal treatment temperature on catalytic performance of Pt/TiO₂ nanobelt composite for HCHO oxidation

CUI Wei-yi^{1, 2
,},
WANG Xi-yue²,
TAN Nai-di^{2
, ,}

1.
The Key Laboratory of Chemical Cleaner Production Technology of Jilin Province, Jilin Institute of Chemical Technology, Jilin 132022, China
2.
College of Chemical and Pharmaceutical Engineering, Jilin Institute of Chemical Technology, Jilin 132022, China

Funds: The project was supported by the National Natural Science Foundation of China (51805207) and 2021 Science and Technology Research and Planning Project of Education Department of Jilin Province (JJKH20210235KJ)

摘要

摘要: 采用水热合成法并结合酸处理制备出TiO₂纳米带，进行不同温度热处理，在TiO₂纳米带上沉积Pt纳米颗粒(NPs)，制备出一系列Pt/TiO₂纳米带复合物，用于甲醛室温催化氧化。通过各种技术对催化剂进行表征，结果表明，热处理温度对TiO₂纳米带的相组成和表面结构，以及表面的氧空位和羟基的数量有较大的影响。在室温下，600 ℃热处理的TiO₂纳米带负载Pt催化剂具有更为丰富的氧空位，有利于吸附氧的活化，并形成较多的Ti-(OH)x-Pt物种，表现出较高的催化活性，在25 ℃，相对湿度为55%时，甲醛的转化率为91.6%。
- 甲醛 /
- 相结构 /
- 热处理温度 /
- 氧空位 /
- 催化氧化
Abstract: TiO₂ nanobelts were prepared by hydrothermal synthesis and acid treatment, then calcination at different temperatures. And subsequently Pt nanoparticles were deposited on the TiO₂ nanobelts. Pt/TiO₂ catalytic properties were investigated in the oxidation of formaldehyde. These catalysts were characterized by various techniques and the characterization results showed that the applied thermal treatment temperature greatly influenced the phase composition and surface structure of TiO₂ nanobelts, as well as the number of oxygen vacancies and hydroxyl groups on the surface. The Pt/TiO₂ nanobelts thermally treated at 600 °C had more oxygen vacancies, which were conducive to the activation of adsorbed oxygen, formed more Ti-(OH)_x-Pt species, and showed higher catalytic activity. At 25 °C and relative humidity of 55%, the conversion of formaldehyde reached 91.6%.
- formaldehyde /
- phase structure /
- thermal treatment temperature /
- oxygen vacancies /
- catalytic oxidation

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FIG. 1067. FIG. 1067.

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图 1 催化剂性能评价流程示意图

Figure 1 Schematic flow diagram of the catalytic performance testing

1: H₂; 2: N₂; 3: O₂; 4,6: flowmeter; 5: HCHO; 7: triple valve; 8: reactor; 9: chromatography; 10: exhaust; 11: carrier gas; 12: off gas

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图 2 Pt/TiO₂催化剂的XRD谱图

a: Pt/TiO₂(A); b: Pt/TiO₂(R); c: PT-C200; d: PT-C300; e: PT-C400; f: PT-C500; g: PT-C600; h: PT-C700

Figure 2 XRD patterns of the Pt/TiO₂ catalysts

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图 3 Pt/TiO₂催化剂的SEM电镜照片

(a): PT-C300; (b): PT-C300; (c): PT-C600; (d): PT-C600

Figure 3 SEM images of Pt/TiO₂ catalyst

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图 4 Pt/TiO₂催化剂的HRTEM电镜照片

(a): PT-C300; (b): PT-C300; (c): PT-C600; (d): PT-C600

Figure 4 HRTEM images of Pt/TiO₂ catalyst

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图 5 TiO₂和Pt/TiO₂的Raman拉曼光谱谱图

a: PT-C600; b: T-C600; c: PT-C300; d: T-C300

Figure 5 Raman spectra of TiO₂ and Pt/TiO₂

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图 6 PT-C300和PT-C600催化剂的XPS谱图

(a)：survey spectra; (b)：Pt 4f; (c)：Ti 2p; (d)：O 1s; a: PT-C300; b: PT-C600

Figure 6 XPS spectra of PT-C300 and PT-C600 catalysts

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图 7 TiO₂和Pt/TiO₂ H₂-TPR谱图

a: T-C300; b: T-C600; c: PT-C300; d: PT-C600

Figure 7 Temperature programmed reduction (H₂ –TPR) profiles of TiO₂ and Pt/TiO₂

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图 8 Pt/TiO₂催化剂的甲醛催化氧化活性

a: PT-C200; b: PT-C300; c: PT-C400; d: PT-C500; e: PT-C600; f: PT-C700; g: Pt/TiO₂(A); h: Pt/TiO₂(R)

Figure 8 HCHO catalytic oxidation activities of the Pt/TiO₂ catalysts

(reaction conditions: HCHO 375 mg/m³, O₂ = 20%, N₂ balance, RH = 55%, GHSV: 60000 cm³/(g·h))

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图 9 PT-C600催化剂的甲醛氧化稳定性

Figure 9 Stability test of PT-C600 for HCHO oxidation (reaction conditions: 25 ℃, HCHO 375 mg/m³, O₂ = 20%, N₂ balance, RH = 55%, GHSV: 60000 cm³/(g·h))

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表 1 Pt/TiO₂催化剂的物化性质和Pt金属分散度

Table 1 Physical properties and Pt dispersion of the Pt/TiO₂ catalyst

Pt/TiO₂ catalyst	A_BET/ (m²·g⁻¹)	Pore volume / (m³·g⁻¹)	Pore size / nm	Pt dispersion/%
PT-C200	81	0.22	8.9	42.2
PT-C300	77	0.22	9.3	40.4
PT-C400	70	0.21	9.7	38.2
PT-C500	64	0.18	11.2	37.2
PT-C600	56	0.16	12.0	37.1
PT-C700	51	0.15	12.5	34.3

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表 2 PT-C300和PT-C600催化剂的XPS分析

Table 2 XPS analysis results for the catalysts of PT-C300 and PT-C600

Catalyst	BE (eV)			Surface atom ratio
Catalyst	Pt 4f_7/2(Pt 4f_5/2)	O_II (O_I)	Ti 2p	O_II /（O_I+ O_II）	Pt/Ti	Pt²⁺/Pt⁰
PT-C300	70.90(74.10)	531.80（529.75）	458.75	0.462	0.041	0.767
PT-C600	70.60(74.00)	531.85（529.80）	458.35	0.618	0.036	0.361
O_Ⅱ/(O_Ⅰ+ O_Ⅱ) and Pt²⁺/Pt⁰ were calculated from the corresponding areas of fitted peaks done by XPSPEAK 4.1 with Shirley background

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