当前位置：
X-MOL 学术
›
Energy Environ. Sci.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
A tailored oxide interface creates dense Pt single-atom catalysts with high catalytic activity
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-01-06 , DOI: 10.1039/c9ee03492g Mi Yoo 1, 2, 3, 4 , Young-Sang Yu 5, 6, 7, 8 , Hyunwoo Ha 1, 2, 3, 4 , Siwon Lee 1, 4, 9, 10 , Jin-Seok Choi 4, 9, 10, 11 , Sunyoung Oh 4, 10, 12, 13, 14 , Eunji Kang 1, 2, 3, 4 , Hyuk Choi 1, 2, 3, 4 , Hyesung An 1, 2, 3, 4 , Kug-Seung Lee 4, 15, 16, 17 , Jeong Young Park 4, 10, 12, 13, 14 , Richard Celestre 5, 6, 7, 8 , Matthew A. Marcus 5, 6, 7, 8 , Kasra Nowrouzi 5, 6, 7, 8 , Doug Taube 5, 6, 7, 8 , David A. Shapiro 5, 6, 7, 8 , WooChul Jung 1, 4, 9, 10 , Chunjoong Kim 1, 2, 3, 4 , Hyun You Kim 1, 2, 3, 4
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-01-06 , DOI: 10.1039/c9ee03492g Mi Yoo 1, 2, 3, 4 , Young-Sang Yu 5, 6, 7, 8 , Hyunwoo Ha 1, 2, 3, 4 , Siwon Lee 1, 4, 9, 10 , Jin-Seok Choi 4, 9, 10, 11 , Sunyoung Oh 4, 10, 12, 13, 14 , Eunji Kang 1, 2, 3, 4 , Hyuk Choi 1, 2, 3, 4 , Hyesung An 1, 2, 3, 4 , Kug-Seung Lee 4, 15, 16, 17 , Jeong Young Park 4, 10, 12, 13, 14 , Richard Celestre 5, 6, 7, 8 , Matthew A. Marcus 5, 6, 7, 8 , Kasra Nowrouzi 5, 6, 7, 8 , Doug Taube 5, 6, 7, 8 , David A. Shapiro 5, 6, 7, 8 , WooChul Jung 1, 4, 9, 10 , Chunjoong Kim 1, 2, 3, 4 , Hyun You Kim 1, 2, 3, 4
Affiliation
|
Highly reactive dense Pt single-atoms stabilized on an oxide support can resolve a grand challenge in the economic use of Pt in catalysis. The maximized number density of reaction sites provided by dense Pt single-atoms guarantees the improved catalytic performance of Pt combined with high efficiency. By manipulating the chemical nature of multi-component interfaces, we synthesized CO-tolerant dense Pt single-atoms highly reactive for the CO oxidation reaction, which governs the key steps for chemical energy conversion and emission control. The addition of 1 wt% of Ce to TiO2 support particles creates a CeOx–TiO2 interface that stabilizes Pt single-atoms by strong electronic interactions. Dense Pt single-atoms formed on CeOx/TiO2 oxides exhibit 15.1 times greater specific mass activity toward CO oxidation at 140 °C compared with a bare Pt/TiO2 catalyst. We elaborate how the CeOx–TiO2 interfaces activate the interface-mediated Mars–van Krevelen mechanism of CO oxidation and protect Pt single-atoms from CO-poisoning. Through a comprehensive interpretation of the formation and activation of dense Pt single-atoms using operando X-ray absorption spectroscopy, density functional theory calculations, and experimental catalyst performance tests, we provide a key that enables the catalytic performance of noble metal single-atom catalysts to be optimized by atomic-scale tuning of the metal–support interface.
中文翻译：
量身定制的氧化物界面可产生具有高催化活性的致密Pt单原子催化剂
稳定在氧化物载体上的高反应性致密Pt单原子可以解决催化中Pt经济使用的巨大挑战。致密的Pt单原子提供的最大反应位密度保证了Pt催化性能的提高和高效率。通过操纵多组分界面的化学性质，我们合成了对CO氧化反应具有高反应性的耐CO的致密Pt单原子，它控制着化学能转换和排放控制的关键步骤。在TiO 2载体颗粒中添加1 wt％的Ce会形成CeO x -TiO 2界面，该界面通过强电子相互作用稳定了Pt单原子。CeO x / TiO上形成致密的Pt单原子2个氧化物表现出对CO氧化，在140℃下用裸铂/二氧化钛相比15.1倍更大的比质量活性2催化剂。我们阐述了CeO x -TiO 2界面如何激活界面介导的Mars-van Krevelen介导的CO氧化机理，并保护Pt单原子免受CO中毒。通过使用操作X射线吸收光谱，密度泛函理论计算和实验催化剂性能测试全面解释致密Pt单原子的形成和活化，我们提供了实现贵金属单原子催化剂催化性能的关键通过对金属-支持界面的原子尺度调整进行优化。
更新日期：2020-01-06
中文翻译：
量身定制的氧化物界面可产生具有高催化活性的致密Pt单原子催化剂
稳定在氧化物载体上的高反应性致密Pt单原子可以解决催化中Pt经济使用的巨大挑战。致密的Pt单原子提供的最大反应位密度保证了Pt催化性能的提高和高效率。通过操纵多组分界面的化学性质，我们合成了对CO氧化反应具有高反应性的耐CO的致密Pt单原子，它控制着化学能转换和排放控制的关键步骤。在TiO 2载体颗粒中添加1 wt％的Ce会形成CeO x -TiO 2界面，该界面通过强电子相互作用稳定了Pt单原子。CeO x / TiO上形成致密的Pt单原子2个氧化物表现出对CO氧化，在140℃下用裸铂/二氧化钛相比15.1倍更大的比质量活性2催化剂。我们阐述了CeO x -TiO 2界面如何激活界面介导的Mars-van Krevelen介导的CO氧化机理，并保护Pt单原子免受CO中毒。通过使用操作X射线吸收光谱，密度泛函理论计算和实验催化剂性能测试全面解释致密Pt单原子的形成和活化，我们提供了实现贵金属单原子催化剂催化性能的关键通过对金属-支持界面的原子尺度调整进行优化。
京公网安备 11010802027423号