1. 西安交通大学动力工程多相流国家重点实验室,西安,710049
2. 中国科学院工程热物理研究所,北京,100190
3. 中国科学院大学航空宇航学院,北京,100049
: 2023-07-10。作者简介: 孙帆(1997—),男,博士生
洪慧(通信作者),女,教授,博士生导师。基金项目: 国家自然科学基金资助项目(51888103)
网络首发:2024-01-10,
纸质出版:2024
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孙帆, 辛宇, 邢学利, 等. 聚光太阳能驱动二氧化碳甲烷化实验研究[J]. 西安交通大学学报, 2024,58(1):89-98.
SUN Fan, XIN Yu, XING Xueli, et al. Experimental Study on Concentrated Solar-Driven CO2 Methanation[J]. 2024, 58(1): 89-98. DOI: 10.7652/xjtuxb202401008.
孙帆, 辛宇, 邢学利, 等. 聚光太阳能驱动二氧化碳甲烷化实验研究[J]. 西安交通大学学报, 2024,58(1):89-98. DOI: 10.7652/xjtuxb202401008.
SUN Fan, XIN Yu, XING Xueli, et al. Experimental Study on Concentrated Solar-Driven CO2 Methanation[J]. 2024, 58(1): 89-98. DOI: 10.7652/xjtuxb202401008. DOI:
针对聚光光热驱动CO
2
甲烷化反应过程中聚光的作用机制尚不清晰的问题
以具有优异反应活性及光热转换特性的Ni/Al
2
O
3
催化剂为研究对象
开展了聚光光热驱动和热驱动下的CO
2
甲烷化实验及机理研究。通过表观活化能测试、温度梯度实验及时间分辨的原位漫反射红外光谱实验
探究了聚光在反应过程中的作用机制
揭示了光热驱动CO
2
甲烷化的反应机理。结果表明
与纯热驱动过程相比
光热驱动在相同温度下表现出更佳的催化性能。光热驱动下w(Ni)为15%的Ni/Al
2
O
3
催化剂在350 ℃下可达到86.8%的CO
2
转化率
达到峰值转化率所需的温度比纯热驱动过程降低了25 ℃。此外
光热较热驱动过程的表观活化能降低了25%
且光致温度梯度进一步促进了CO
2
的转化。时间分辨的原位漫反射红外光谱实验结果表明
聚光改善了CO
2
在催化剂表面的吸附
促进了关键中间体的转变
增强了CO
*
生成CH
4
的反应路径
从微观动力学上促进了CO
2
的转化。该研究为认识聚光太阳能驱动CO
2
甲烷化过程中聚光的作用机制提供了新的思路。
This study investigates the mechanism of concentrated light in the photothermal CO
2
methanation process using a highly reactive Ni/Al
2
O
3
catalyst with excellent photothermal conversion characteristics experimental investigations were performed under concentrated photothermal and thermal driven conditions to shed light on the reaction mechanism. Apparent activation energy tests
temperature gradient experiments and time-resolved in-situ diffuse reflectance infrared spectroscopy experiments were c
onducted
to gain insights into the process. The results demonstrate that the photothermal-driven process outperforms the thermal-driven process
exhibiting superior catalytic performance at the same temperature. Remarkably
a Ni/Al
2
O
3
catalyst containing 15% mass fraction of Ni achieved an impressive CO
2
conversion rate of 86.8% at 350 ℃ under the photothermal-driven condition. Notably
the photothermal-driven process required a 25 ℃ lower temperature to achieve the highest CO
2
conversion rate compared to the thermal-driven process. The apparent activation energy of the photothermal-driven process was reduced by 25%
and the concentrated light-induced temperature gradient further enhanced CO
2
conversion. Time-resolved in-situ diffuse reflectance infrared spectroscopy experiments showed that concentrated light improved CO
2
adsorption on the catalyst surface
promoted the transformation of key intermediates
and enhanced the reaction pathway of CO
*
to CH
4
thereby enhancing CO
2
conversion at a microscopic level. This study provides valuable insights into the role of concentrated light in CO
2
methanation driven by concentrated solar energy
shedding light on the underlying mechanism.
International Energy Agency. CO2甲烷化镍基催化剂研究进展 [J]. 洁净煤技术, 2022, 28(4): 1-17.ZHANG Xiaoli, GU Fangna, SU Fabing, et al. Research progress of nickel-based catalysts for carbon dioxide methanation [J]. Clean Coal Technology, 2022, 28(4): 1-17.
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