钴等离激元超结构粉体催化剂的制备及其光热催化应用

doi:10.15541/jim20210458

无机材料学报 ›› 2022, Vol. 37 ›› Issue (1): 22-28.DOI: 10.15541/jim20210458

所属专题：【能源环境】CO2绿色转换

• 专栏: CO ₂ 绿色转化(特邀编辑: 欧阳述昕, 王文中) • 上一篇下一篇

钴等离激元超结构粉体催化剂的制备及其光热催化应用

王潇(), 朱智杰, 吴之怡, 张城城, 陈志杰, 肖梦琦, 李超然(), 何乐()

苏州大学功能纳米与软物质研究院, 江苏省碳基功能材料与器件重点实验室, 苏州 215000

收稿日期:2021-07-19 修回日期:2021-08-23 出版日期:2022-01-20 网络出版日期:2021-08-20
通讯作者: 何乐, 教授. E-mail: lehe@suda.edu.cn; 李超然, 副研究员. E-mail: crli@suda.edu.cn
作者简介:王潇(1997-), 女, 硕士研究生. E-mail: 20194214065@suda.stu.cn
基金资助:
国家自然科学基金(51802208);国家自然科学基金(21902113);国家自然科学基金(52172221)

Preparation and Photothermal Catalytic Application of Powder-form Cobalt Plasmonic Superstructures

WANG Xiao(), ZHU Zhijie, WU Zhiyi, ZHANG Chengcheng, CHEN Zhijie, XIAO Mengqi, LI Chaoran(), HE Le()

Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou 215000, China

Received:2021-07-19 Revised:2021-08-23 Published:2022-01-20 Online:2021-08-20
Contact: HE Le, professor. E-mail: lehe@suda.edu.cn; LI Chaoran, associate professor. E-mail: crli@suda.edu.cn
About author:WANG Xiao(1997-), female, Master candidate. E-mail: 20194214065@suda.stu.cn
Supported by:
FundNational Natural Science Foundation of China(51802208);FundNational Natural Science Foundation of China(21902113);FundNational Natural Science Foundation of China(52172221)

摘要/Abstract

摘要：

高吸光催化剂对提高光热转换效率具有重要意义, 阵列结构光热催化剂的陷光效应有助于增强光吸收并提高光热转换效率。但是, 现有阵列基光热催化剂仍存在单位面积上活性金属负载量过低的不足, 难以满足实际应用的需求。本研究发展了二氧化硅保护的MOFs热解策略, 获得了单位辐照面积上活性金属质量可调、太阳光吸收效率超过90%的粉体钴等离激元超结构光热催化剂, 通过时域有限差分法模拟计算证实其高吸光能力源于纳米颗粒的等离子杂化效应。相比阵列基等离子体超结构催化剂, 该粉体结构的催化活性和稳定性显著增强, 在相同催化条件下, 二氧化碳转化率从0.9%提高到26.2%。本研究为非贵金属光热催化剂的实际应用奠定了基础。

关键词: 光热催化, 二氧化碳加氢, 等离子体超结构, 高吸光催化剂, 光-化学能转换

Abstract:

Highly light absorptive photocatalysts are of great significance to boost the photothermal conversion efficiency. Light trapping effect of nanoarray structured photothermal catalysts can enhance the light absorption and improve the photothermal conversion efficiency. However, the practical applications of array-based catalysts are hindered by very low loadings of active metal catalysts per unit illumination area. Herein, we develop a SiO₂-protected MOFs pyrolysis method for the preparation of powder-form cobalt plasmonic superstructures that enable a 90% absorption efficiency of sunlight and tunable metal loading per unit area. Its high light absorption capacity was confirmed by time-domain finite-difference simulation calculations due to the plasmonic hybridization effect of nanoparticles. Compared with nanoarray-structured plasmonic superstructures, the powder-form catalyst exhibit enhanced catalytic activity and stability, resulting in the increase of CO₂ conversion efficiency from 0.9% to 26.2%. This study lays the foundation for the practical application of non-precious metal photothermal catalysts.

Key words: photothermal catalysis, carbon dioxide hydrogenation, plasmonic superstructure, strong light absorptive catalyst, solar-to-chemical energy conversion

中图分类号:

TQ174

王潇, 朱智杰, 吴之怡, 张城城, 陈志杰, 肖梦琦, 李超然, 何乐. 钴等离激元超结构粉体催化剂的制备及其光热催化应用[J]. 无机材料学报, 2022, 37(1): 22-28.

WANG Xiao, ZHU Zhijie, WU Zhiyi, ZHANG Chengcheng, CHEN Zhijie, XIAO Mengqi, LI Chaoran, HE Le. Preparation and Photothermal Catalytic Application of Powder-form Cobalt Plasmonic Superstructures[J]. Journal of Inorganic Materials, 2022, 37(1): 22-28.

图/表 7

图1 Co-SiO2催化剂制备与表征

Fig. 1 Preparation and characterization of Co-SiO2 (a) Schematic illustration of preparation of Co and Co-SiO2 catalysts, TEM images of (b) ZIF-67-SiO2, (c) Co and (d) Co-SiO2, (e) HRTEM, (f) SAED and (g-j) elemental mappings of Co-SiO2

图2 (a)ZIF-67和ZIF-67-SiO2的XRD谱图, (b)Co和Co-SiO2的XRD图谱

Fig. 2 XRD patterns of (a) ZIF-67, ZIF-67-SiO2, and (b) Co and Co-SiO2

图3 (a)Co-SiO2和Co的漫反射光谱, 插图为Co-SiO2和Co催化剂的实物图; (b)不同Co颗粒堆积的归一化消光系数模拟图; 红外相机观测的 (c)Co催化剂与(d)Co-SiO2催化剂的表面平均温度

Fig. 3 (a) Diffuse reflectance spectra of Co-SiO2 and Co (insets showing photographs of two catalysts), (b) dependence of calculated normalized extinction cross-section of Co nanostructures on the number of Co nanoparticles (n) in the chain, and surface temperature of (c) Co catalyst and (d) Co-SiO2 catalyst

图4 催化剂在不同光强下的催化活性和CO选择性图

Fig. 4 Catalytic activity and CO selectivity of Co-SiO2 under different light intensities

表1 不同催化剂在光热二氧化碳加氢反应中的CO2转化率

Table 1 CO2 conversion efficiencies of different catalysts in photothermal hydrogenation of carbon dioxide

Sample	Metal mass per unit area /(mg·cm^-2)	Size of Co/nm	CO₂ conversion /%	CO selectivity /%
Co-SiO₂-1	0.41	27	11.9	61.0
Co-SiO₂-2	0.86	27	17.6	34.9
Co-SiO₂-3	1.4	27	26.2	29.7
Co-SiO₂-4	1.7	27	24.8	27.2
Co-PS@SiO₂	0.32	25	0.9	70.4

图5 Co-SiO2和Co在300 ℃连续工作4 h内的热催化二氧化碳加氢稳定性比较

Fig. 5 Stability of Co-SiO2 and Co in thermocatalytic CO2 hydrogenation at 300 ℃ (a) CO2 conversion rate; (b) CO selectivity

图6 催化测试后的Co-SiO2的(a)TEM照片及其(b)粒径统计

Fig. 6 (a) TEM image and (b) particle size distribution of spent Co-SiO2

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钴等离激元超结构粉体催化剂的制备及其光热催化应用

Preparation and Photothermal Catalytic Application of Powder-form Cobalt Plasmonic Superstructures

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