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Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity
Advanced Science ( IF 14.3 ) Pub Date : 2017-07-25 , DOI: 10.1002/advs.201700252
Jia Jia 1 , Hong Wang 2 , Zhuole Lu 3 , Paul G O'Brien 4 , Mireille Ghoussoub 2 , Paul Duchesne 5 , Ziqi Zheng 2 , Peicheng Li 1 , Qiao Qiao 6, 7 , Lu Wang 2 , Alan Gu 3 , Abdinoor A Jelle 2 , Yuchan Dong 2 , Qiang Wang 8 , Kulbir Kaur Ghuman 1 , Thomas Wood 3 , Chenxi Qian 2 , Yue Shao 2 , Chenyue Qiu 1 , Miaomiao Ye 9 , Yimei Zhu 6 , Zheng-Hong Lu 1 , Peng Zhang 5 , Amr S Helmy 10 , Chandra Veer Singh 1 , Nazir P Kherani 1, 10 , Doug D Perovic 1 , Geoffrey A Ozin 2
Affiliation  

This study has designed and implemented a library of hetero‐nanostructured catalysts, denoted as Pd@Nb2O5, comprised of size‐controlled Pd nanocrystals interfaced with Nb2O5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb2O5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH4 production rates as high as 0.75 and 0.11 mol h−1 gPd−1, respectively. By contrast, using small Pd nanocrystals, a CO production rate surpassing 18.8 mol h−1 gPd−1 is observed with 99.5% CO selectivity. These performance metrics establish a new milestone in the champion league of catalytic nanomaterials that can enable solar‐powered gas‐phase heterogeneous CO2 reduction. The remarkable control over the catalytic performance of Pd@Nb2O5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.

中文翻译:

光热催化剂工程:高活性和定制选择性的气态 CO2 加氢

本研究设计并实现了异质纳米结构催化剂库,表示为 Pd@Nb 2 O 5 ,由与 Nb 2 O 5纳米棒连接的尺寸受控的 Pd 纳米晶体组成。该研究还表明,可以通过改变Nb 2 O 5纳米棒上负载的Pd纳米晶体的尺寸来系统地调整CO 2还原成CO和CH 4产物的催化活性和选择性。使用大的Pd纳米晶体,该研究实现了CO和CH 4生产率分别高达0.75和0.11 mol h -1 g Pd -1。相比之下,使用小Pd纳米晶体,观察到超过18.8 mol h -1 g Pd -1的CO生产率,CO选择性为99.5%。这些性能指标在催化纳米材料冠军联赛中树立了新的里程碑,可以实现太阳能驱动的气相多相CO 2还原。事实证明,对Pd@Nb 2 O 5催化性能的显着控制源于光热效应、电子效应和尺寸效应的结合,这些效应可以通过纳米化学合理调节。
更新日期:2017-07-25
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