ChemCatChem
·
2021
·Vol. 13
·期 21
·4610-4617
·
IF 5.686
Yifei Yang,Linsen Zhou,Jun Chen,Ruizhi Qiu,Yunxi Yao
Graphical Highly dispersed Pt clusters supported on TiN substrates favor the formation of highly reactive dual sites. Molecular O 2 dissociatively adsorbs on the Ti−Ti bridge sites to form titanium oxynitride (TiN x O y ) skin and the oxygen atom binding on Ti sites readily react with the adjacent CO adsorbed on Pt to attain the catalytic cycle. The interfacial synergistic effect between Pt and TiN results in superior performance in the low-temperature CO oxidation. The metal-support interfacial synergistic catalysis allows the competitive reaction steps to occur in close proximity at different sites, thus decreasing the activation barrier and improving the catalytic efficiency. Combining the structural characterization, reactivity assessments and density functional theory (DFT) calculations, it is found that highly dispersed Pt clusters on TiN substrates favor the formation of Pt−TiN interfacial dual sites, which are highly reactive for the low-temperature CO oxidation with an apparent activation energy as low as 38.7 kJ mol −1 , much less than that on the traditional Pt/TiO 2 or Pt/SiO 2 catalysts. At low temperature, the surface sites of Pt are saturated with CO adsorption due to its high adsorption energy and the molecular O 2 dissociatively adsorbs on the Ti sites to form the titanium oxynitride (TiN x O y ) skin with a low barrier of 0.1 eV. The O atoms binding on Ti sites readily react with the adjacent CO molecules adsorbed on the perimeter of Pt clusters to attain a catalytic cycle with a reaction barrier of 0.5 eV. The interfacial synergistic effect between Pt and TiN is the origin of the low temperature CO oxidation activity on the metal-nitride catalysts.
研究领域:
催化
·
材料科学
·
化学工程
·
表面化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Hongbing Wang,Yifei Yang,Linsen Zhou,Jun Chen,Linan Lin,Xinchun Mao,Wei Cui,Yunxi Yao
The reactive interfacial sites upon supported catalysts provide an alternative pathway to enable the reactants activation in an energetically favorable mode, thus decreasing the energy barrier and promoting the catalytic efficiency. By virtue of structural characterization, in-situ spectroscopic analysis, kinetic assessments and density functional theory (DFT) calculations, supported Pt/TiN catalysts are systematically studied to interrogate H 2 O activation on the Pt-TiN interfacial sites and its catalytic function during the low-temperature water gas shift (WGS). It is found that the partially oxygen-covered TiN surface is highly efficient for H 2 O activation by oxygen-assisted dissociation with an energy barrier of 0.41 eV, much less than that on metallic Pt surface. The formed hydroxyls binding on Ti sites, observed by in-situ X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD), could readily react with the adjacent CO adsorbed on Pt clusters with the reaction energy barrier of 0.43 eV to attain the individual catalytic cycle. Benefiting from the enhanced H 2 O activation, the catalytic turnover rate of CO-H 2 O reaction on Pt/TiN is 3.8 and 20.3 times higher than that on traditional Pt/TiO 2 and Pt/SiO 2 at 403 K, respectively. The interfacial reactive sites are the origin of low-temperature WGS on Pt/TiN catalysts.
研究领域:
催化
·
材料科学
·
化学工程
·
表面化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xuan Yu,Xu Liu,Jinyan Zhao,Mingzhe Xue,Huaijie Shi,Chenghang Jiang,Jia Liu,Yufeng Xue,Fengying Gao,Xing Zhong,Zihao Yao,Jianguo Wang
Electrochemical ozone production (EOP) is a technology with great promise for ozone synthesis, where electrochemical anode and cathode reactions play key roles in electrolytic ozone generators. In this work, mesoporous three-dimensional Pt/TiN nanorods (NRs) have been designed and prepared for EOP and HER, exhibited impressive performance with the faraday efficiency of the anodic EOP was 13 %. The overpotential of cathodic HER was 38 mV at 10 mA·cm −2 with 0.5 M H 2 SO 4 . The porous structure of Pt/TiN NRs provides microenvironments favorable for enrichment of reaction intermediates, accelerating the kinetic processes of EOP and HER. Theoretical calculations have revealed that metal-support interactions (MSI) between Pt and TiN play an influential role in the adsorption of reactive intermediates. Furthermore, promising efficiencies in the electrochemical degradation of organic pollutants have been investigated, highlighting the potential application of the Pt/TiN NRs-1 || Pt/TiN NRs-2 in advanced electrochemical oxidation.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2024
·Vol. 35
·期 38
·385705
·
IF 2.9
Yongguang Xiao,Lisha Yang,Yong Jiang,Siwei Liu,Gang Li,Jun Ouyang,Minghua Tang
Lu doped Hf0.5Zr0.5O2 (HZO) ferroelectric films were prepared on Pt/TiN/SiO2/Si substrate by chemical solution deposition method, and an interfacial engineering strategy for improving the ferroelectric property was explored by capping the Lu doped HZO films with a cerium oxide layer. Compared with the Lu doped HZO film without the CeOx coating layer, the Lu doped HZO film with the CeOx coating layer has a larger remanent polarization (2Pr = 34.72 µC cm−2) and presents weaker wake-up behavior, which result from the higher orthogonal phase ratio and the lower oxygen vacancy of the CeOx coated Lu doped HZO film. In addition, the CeOx coating can remarkably improve the fatigue resistance and retention performance of the Lu doped HZO films. It is hoped that the results can provide an effective approach for the realization of high-performance and highly reliable hafnium oxide based ferroelectric thin films.
研究领域:
材料科学
·
铁电材料
·
薄膜
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Hui Song,Jinshu Wang,Xinxin Wang,Guangshun Ran,Chunxia Lin,Tianjiao Lou,Jinxu Song,Xing Cheng,Wenyuan Zhou,Hongyi Li
Efficient hydrogen evolution at high current densities requires simultaneous optimization of intrinsic reaction kinetics, multiphase mass transport, and electrode durability. Here, we constructed a binder-free Pt/TiN NTs@3D-TC4 electrode by integrating Pt nanoparticles and in situ-grown TiN nanotube arrays on a three-dimensional printed porous titanium-alloy scaffold. Its high performance arises from three mutually reinforcing effects. First, the work function mismatch between Pt and TiN drives electron transfer from TiN to Pt, producing electron-rich Pt sites and an interfacial built-in electric field. Combined with Pt–N coordination and d - p orbital hybridization, this electronic metal-support interaction optimizes hydrogen adsorption and desorption energetics, thereby enhancing intrinsic hydrogen evolution reaction activity. Second, the periodic macroporous scaffold and nanoparticle-assembled TiN nanotubes create a superhydrophilic and aerophobic multiscale transport network. This network promotes electrolyte infiltration, proton delivery, and rapid bubble detachment while mitigating gas shielding at high current densities. Third, robust Pt–N anchoring and binder-free integration of the catalytic layer with the conductive framework suppress Pt migration, aggregation, and detachment. Consequently, Pt/TiN NTs@3D-TC4 requires overpotentials of only 30.8 and 207 mV to deliver 10 and 1000 mA cm −2 , respectively. It also achieves a Pt mass activity of 20.81 A mg Pt −1 at 200 mV and operates stably for over 200 h at 1 A cm −2 . These results establish a practical electrode design that combines hierarchical transport regulation with interfacial electronic modulation for scalable hydrogen production at high current densities. Interfacial electron transfer optimizes H* adsorption/desorption; multiscale hydrophilic architecture accelerates bubble release and mass transport; Pt–TiN interaction ensures structural stability. The triple enhancement enables scalable, high-current-density water electrolysis. Download: Download high-res image (145KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
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