JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Zhao Yang,Wenhan Chen,Jinbao Zheng,Zhiqing Yang,Nuowei Zhang,Chuan-Jian Zhong,Bing Hui Chen
Carbon supported Pt-Ru nano-alloy with multiple reactive sites exhibits unprecedentedly efficient performance in acetone hydrogenation at room temperature. Catalytic properties can be controllably regulated and optimized via performing the specific annealing treatment for the catalyst. The essential correlation between the variations in catalyst’s annealing conditions and the resultant variation in catalytic properties has been explored and discussed as a structure-function relationship. The combination of Pt and Ru sites exhibits enhanced catalytic activity compared with monometallic ones. Larger PtRu alloy particle size favors the rapid C O hydrogenation and the improvement of catalytic selectivity to isopropanol. Isopropyl ether generation is related to the Pt defect sites on the surface, which can be blocked though the catalyst’s oxidation treatment . The presence of surface metal-oxide species is beneficial to the performance enhancement, resulting from the synergetic behavior between metal-oxide sites and metallic sites on respectively activating the reactants. Moreover, 3-pentanone is used as a probe molecule to verify the structure-function relationship of catalytic low-temperature C O hydrogenation on PtRu/C.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Haiyang Wang,Caiyan Gao,Zhongyi Liu,Baojun Li,Young Dok Kim,Jie Feng,Kaihang Sun,Zhikun Peng
Active and durable electrocatalysts are essential for commercializing direct methanol fuel cells. However, Pt-based catalysts, extensively utilized in the methanol oxidation reaction (MOR), are suffered from resource scarcity and CO poisoning, which degrade MOR activity severely. Herein, Pt 1 Ru x bimetallic catalysts were synthesized by confining Pt 1 Ru x alloys within the shells of mesoporous carbon hollow spheres (MCHS) via a vacuum-assisted impregnation method (Pt 1 Ru x @MCHS). The confinement effect induced by mesoporous carbon hollow spheres resulted in a robust structure of Pt 1 Ru 3 @MCHS with an ultrafine dispersion of alloy nanoparticles. The experimental and theoretical results confirmed that the boosting electrocatalytic activity and stability of the MOR over Pt 1 Ru 3 @MCHS were contributed to the regulated electronic structure as well as the superior CO tolerance of atomic Pt site caused by the electronic interaction between single Pt atoms and Ru nanoparticles. This strategy is versatile for the rational design of Pt-based bimetallic catalysts and has a positive impact on MOR performance.
研究领域:
材料科学
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电化学
·
纳米技术
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能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 40
·13999-14008
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IF 4.174
Mingxuan Li,Yao Wang,Jing Cai,Yunrui Li,Yujie Liu,Yin Dong,Shuna Li,Xiaolin Yuan,Xin Zhang,Xiaoping Dai
Modifying the surface active sites of Pt-based catalysts at the atomic level is of great significance to enhance the electrooxidation of methanol molecules. Herein, efficient active site assembly strategies are proposed, precisely, aimed at building high-performance electrocatalysts. Serving as proof-of-concept examples, both instances of Pt nanowires surface doping isolated Ru atoms (Ru/Pt NWs) and Ru nanoparticles supported on Pt nanowires (Ru@Pt NWs) are specially designed to optimize the catalytic performance of methanol oxidation reaction (MOR). The specific activity and mass activity of optimal Ru/Pt NWs can reach up to 3.93 mA cm−2 and 568.40 mA mg−1Pt, respectively, which is 1.53/1.94 times that of the Ru@Pt NWs and 2.03/2.59 times that of pure Pt NWs. Detailed studies on mechanism reveal that the Pt–Ru alloy can significantly improve the electron transfer kinetics of MOR, and activate more Pt atoms involved in the Langmuir–Hinshelwood (L–H) pathway compared with Ru@Pt NWs, all of which collectively accelerate the methanol oxidation. This surface engineering strategy via assembling active sites can reveal a promising method in the design of advanced Pt-based catalysts for direct methanol fuel cells.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Catalysis
·
2022
·Vol. 5
·期 10
·900-911
·
IF 40.706
Li Peng,Jiang Yaling,Hu Youcheng,Men Yana,Liu Yuwen,Cai Wenbin,Chen Shengli
The origin of the large kinetic pH effect in hydrogen electrocatalysis, that is, the approximately two orders of magnitude decrease in reaction kinetics when moving from acid to alkaline, remains far from having a consensus. Here we show that it is the significantly different connectivity of hydrogen-bond networks in electric double layers that causes the large kinetic pH effect. This result has been obtained by meticulously comparing the electric double layers of acid and alkaline interfaces from ab initio molecular dynamics simulations, and the computed vibrational density of states of water molecules in the interfaces simulated with ab initio molecular dynamics, with the results of in situ surface-enhanced infrared absorption spectroscopy. Using a Pt–Ru alloy as a model catalyst, we further reveal an unanticipated role of OH adsorption in improving the kinetics of alkaline hydrogen electrocatalysis, namely, by increasing the connectivity of hydrogen-bond networks in electric double layers rather than by merely affecting the energetics of surface reaction steps. These findings highlight the key roles of electric double layer structures in electrocatalysis.
研究领域:
电化学
·
催化
·
材料科学
·
表面科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）