JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Rundong Ma,Han Tian,Xu Yu,Xiangzhi Cui,Xinmei Hou,Shengli An
Hydrogen oxidation reaction (HOR) as the anode reaction in proton exchange membrane fuel cell, usually suffers from the high loading of platinum (Pt) and subsequent CO poisoning especially by using industrial crude hydrogen as fuel. In this work, we propose a directional electron transfer route from Pt to MoO 2- x in the macroporous structure to significantly enhance the HOR activity as well as the CO tolerance, which is constructed by interface engineering and defect strategy to anchor highly dispersed Pt nanoparticles onto the three-dimensional MoO 2- x -C framework. The optimized 2Pt-MoO 2- x -C with 1.02 wt% Pt demonstrates higher HOR peak current density (3.57 mA cm −2 ) and nearly 25 times higher mass activity than 20 wt% Pt/C. The excellent HOR performance is attributed to the synergistic effect between Pt and MoO 2- x species, in which the charge transfer from Pt to MoO 2- x improves H 2 adsorption ability of Pt and accelerates the activation of H 2 due to the reduced hydrogen binding energy of MoO 2- x caused by Pt-O construction, leading to the release of H* thereby the enhancement of HOR activity. The construction of three-dimensional macroporous structure enhances the HOR dynamics by promoting the conductivity, mass transfer and the exposure of active sites. Moreover, the formed Mo-OH in Pt-MoO 2- x -C can effectively react with CO species to remove the CO poisoning of Pt, endowing the excellent CO tolerance.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Yu Cao,Pei Liang,Qianmin Dong,Dan Wang,De Zhang,Lisha Tang,Le Wang,Shangzhong Jin,Dejiang Ni,Zhi Yu
Recently, more and more attention has been given to a semiconductor oxide-based surface-enhanced Raman spectroscopy substrate for its great stability and biocompatibility. However, its poor SERS sensitivity limits the applications of semiconductor oxide SERS substrates. In this paper, we provide a facile reduction method to modulate oxygen vacancy concentrations in oxide SERS substrates. Using MoO2 as an example, the resonance coupling as well as charge transfer between the semiconductor oxide SERS substrate and the target molecules were promoted for the reason of artificial oxygen vacancy embodied in the Raman signals being improved. By using the TEM, SEM, and XPS measurements, we confirmed that we successfully prepared defective MoO2–x with a polycrystalline surface. MoO2–x modulated oxygen vacancy treated with 6 wt % Li shows a very high detection sensitivity of 10–8 M (4.79 ug/L) for R6G, and the intensity of the Raman signal was highly enhanced. Because of the existence of defective energy levels, resonance coupling, as well as charge transfer between semiconductor and molecules, was obviously promoted. More importantly, the method of modulating oxygen vacancy can be widely used in semiconductor oxide materials for its chemical enhancement capacity can be promoted by artificial oxygen vacancy.
研究领域:
材料科学
·
光谱学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Jia Sun,Chunyu Zhang,Hang Song,Yu Kang,Zhenqing Zhang,Yujia Han,Lu Shang,Lixue Zhang,Xiaoli Yang,Yi Cui
The sluggish water dissociation kinetics and suboptimal hydrogen adsorption on Ru-based catalysts remain major challenges for efficient alkaline hydrogen evolution reaction (HER). Constructing spatially coupled yet functionally distinct active sites through metal-support interaction (MSI) offers a promising route to overcome these intrinsic kinetic limitations. Herein, a pathway-controlled defect engineering strategy is developed, in which carbon is introduced in situ during oxide reduction to generate oxygen-vacancy-rich MoO 2− x supports and thereby establish strong MSI with Ru. Structural and spectroscopic analyses reveal that oxygen vacancies in MoO 2− x preferentially adsorb and activate interfacial water, while defect-mediated MSI electronically modulates Ru to optimize *H binding. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory calculations collectively demonstrate that this interfacial synergy induces strong water-support interactions, effectively lowering the Volmer-step energy barrier under alkaline conditions. As a result, Ru/C-MoO 2− x -800 delivers outstanding alkaline HER performance, achieving an overpotential of 23 mV at 10 mA cm −2 with a Tafel slope of 35 mV dec −1 . The catalyst sustains stable operation for 1000 h at an application-relevant current density of 250 mA cm −2 in an anion exchange membrane water electrolyzer (AEMWE). This work establishes defect-regulated MSI as an effective design principle for decoupling water activation and hydrogen adsorption in alkaline HER. Tailored oxygen vacancy engineering strengthens Ru-MoO 2− x metal-support interactions and regulates interfacial water activation and hydrogen adsorption energetics, enabling efficient and durable alkaline hydrogen evolution. Download: Download high-res image (210KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Zhian Chen,Yi Shu,Xia Gui,Nengcong Yang,Yunfei Li,Saidi Qi,Song Sun,Haiqun Cao,Sheng Ye,Chunyan Zhang
The production of high-value chemicals from renewable biomass carbon resources represents a critical pathway toward sustainable development. However, this process is often constrained by harsh reaction conditions and low selectivity. Herein, we design an oxygen vacancy (OV)-rich MoNi3/MoO2+x heterostructure catalyst, which exhibited superior performance in a neutral phosphate buffer (pH = 7), with an anodic reaction selectivity of 95% for the biomass derived benzylamine oxidation to N-benzylidene benzylamine and a low overpotential of 64 mV at 10 mA cm–2 for cathode H2 evolution. The high selectivity was achieved by tuning •OH coverage through the precise construction of a unique interface between OV-rich amorphous MoO2+x and metallic MoNi3. Moreover, the dual electrode system operated stably for 150 h at 10 mA cm–2 under an applied voltage of only 1.53 V. This work provides an effective approach for the green production of high-value imines and H2 by synergistic vacancy and interfacial engineering.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）