Light assisted CO2 reduction with methane over SiO2 encapsulated Ni nanocatalysts for boosted activity and stability
Light assisted CO2 reduction with methane over SiO2 encapsulated Ni nanocatalysts for boosted activity and stability
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在 SiO2 封装的 Ni 纳米催化剂上用甲烷光辅助还原 CO2，以提高活性和稳定性
DOI：
10.1039/c7ta00704c
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发表时间：
2017-05
影响因子：
11.9
通讯作者：
Ye Jinhua
中科院分区：
文献类型：
--
作者：
Liu Huimin;Meng Xianguang;Thang Duy Dao;Liu Lequan;Li Peng;Zhao Guixia;Nagao Tadaaki;Yang Liuqing;Ye Jinhua
在这项研究中，地球丰富的甲烷作为还原剂的CO2光还原（CRM）的能量存储。将光引入热驱动反应体系，旨在改善催化剂在低温下的催化性能。首次将不同形貌的镍基纳米催化剂应用于光辅助CRM，观察到了一些有趣的现象。一个是，与光照射，提高初始催化活性观察到所有的Ni纳米催化剂。Ni的等离子体性质和带间跃迁产生的热电子促进了反应物的活化，并参与了初始活性的提高。另一个现象是，在光照射下，可以观察到蛋黄-壳Ni@SiO2-蛋黄和核-壳Ni@SiO2-核催化剂的改善的稳定性。对废催化剂的表征表明，在光照射下，石墨化结构的催化剂上石墨碳的沉积量随活性炭沉积量的减少而增加，而活性炭沉积量的减少是催化剂稳定性提高的主要原因。据我们所知，本研究首次报道了光照射可以影响碳的形成行为，同时，它提供了一种方法，以提高在CO2光还原纳米催化剂的活性和稳定性。
In this study, earth-abundant methane was adopted as the reductant in CO2 photoreduction (CRM) for energy storage. Light was introduced into the thermally driven reaction system with the aim to improve the catalytic performance of catalysts at low temperatures. Ni-based nanocatalysts of different morphologies were first adopted in light assisted CRM and some interesting phenomena were observed. One is that, with light irradiation, boosted initial catalytic activities were observed over all the Ni nanocatalysts. Hot electrons resulted from Ni plasmonic property and interband transition facilitated reactant activation and participated in the initial activity enhancement. Another phenomenon is that improved stability could be observed over yolk–shell Ni@SiO2-yolk and core–shell Ni@SiO2-core catalysts with light irradiation. Characterization of the spent catalysts revealed that, over the encapsulation-structured catalysts, with light irradiation, the amounts of deposited graphitic carbon increased with the sacrifice of active carbon deposition, and the smaller amount of detrimental active carbon deposition was regarded to be responsible for the improved stability. To the best of our knowledge, this study for the first time reports that light irradiation could exert effects on carbon formation behavior; meanwhile, it offers an approach to improve the activity and stability of nanocatalysts in CO2 photoreduction.
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影响因子：
4
作者：
Bower, C;Zhou, O;Jin, SH
通讯作者：
Jin, SH
影响因子：
22.1
作者：
Boukha, Zotihair;Jimenez-Gonzalez, Cristina;Lopez-Fonseca, Ruben
通讯作者：
Lopez-Fonseca, Ruben
影响因子：
7.3
作者：
Chen, Y;Ciuparu, D;Pfefferle, L
通讯作者：
Pfefferle, L
影响因子：
3.7
作者：
Ferrari, AC;Robertson, J
通讯作者：
Robertson, J
影响因子：
5.3
作者：
Weiwei Yang;Huimin Liu;Yuming Li;Juan Zhang;Hao Wu;Dehua He
通讯作者：
Weiwei Yang;Huimin Liu;Yuming Li;Juan Zhang;Hao Wu;Dehua He