Journal of Materials Chemistry A
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2023
·Vol. 12
·期 6
·3565-3574
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IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 14
·8567-8574
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IF 3.108
Jiachun Chai,Shanhui Zhu,Youliang Cen,Jing Guo,Jianguo Wang,Weibin Fan
One-pot hydrogenolysis of cellulose to ethylene glycol (EG) was carried out on WO3-based catalysts combined with Ru/C. To probe the active catalytic site for breaking the C–C bond of cellulose, a series of WO3–ZrO2 (WZr) catalysts were synthesized and systematically characterized with XRD, Raman, UV-Vis, H2-TPR, DRIFS and XPS techniques and N2 physisorption experiment. It was found that the WO3 crystallites became more easily reduced to W5+–OH species with increasing crystallite size or tungsten surface density of the WZr catalyst owing to the decrease of their absorption edge energy (AEE) originating from weakening their interaction with ZrO2 support. This, as a result, gave higher EG yield at higher tungsten surface density. The structure–activity relationship of the WZr catalyst reveals that the active catalytic site for cleaving the C2–C3 bond of the glucose molecule is the W5+–OH species.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Catalysis
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2020
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IF 12.35
Yang Chen,Yingxin Feng,Lin Li,Jingyue Liu,Xiaoli Pan,Wei Liu,Fenfei Wei,Yitao Cui,Botao Qiao,Xiucheng Sun,Xiaoyu Li,Jian Lin,Sen Lin,Xiaodong Wang,Tao Zhang
Exclusive Pt species supported on inert substrates have not achieved satisfactory performance for cryogenic CO oxidation because of the constraint of the competitive Langmuir–Hinshelwood process in which the strongly adsorbed CO inhibits the activation of O2. Here, we develop a catalyst of Pt nanoparticles on Al2O3 that exhibits extremely high activity with 100% CO conversion at −20 °C and orders of magnitude higher specific rate than current commercial catalysts. Detailed catalyst characterizations reveal the presence of metallic Pt sites and positively charged ones associated with the OH species in Pt/Al2O3. Both experimental data and theoretical calculations suggest that CO adsorbed on Pt(OH) kink sites reacts with OH species covering Pt0 terrace sites to release CO2. Afterward, O2 is facilely activated on terrace sites to regenerate OH. The presence of OH species and the synergy between Pt kink and terrace sites on the Pt species lead to an ultralow reaction barrier for CO oxidation.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Chunyu Zhang,Guang Yang,Xueqing Gao,Zhiyun Li,Yifan Li,Siyuan Wang,Junyong Wang,Xunhua Zhao,Kai Zhang,Yu Kang,Yi Cui
Surface OH species on electrocatalysts play a pivotal role in affecting the hydrogen evolution reaction (HER). Herein, we highlight the critical role of surface OH basicity in regulating interfacial water structure and OH desorption behavior. By annealing Ru/Ni(OH) 2 at various temperatures, we successfully tailored the electronic state of surface OH species, with the catalyst annealed at 300 °C (Ru-Ni-300) exhibiting superior HER performance, achieving a current density of 100 mA/cm 2 at an exceptionally low overpotential of 71 mV. X-ray photoelectron spectroscopy demonstrates that the electron-rich surface OH species on Ru-Ni-300 exhibit strong Lewis basicity. The enhanced OH basicity facilitates the formation of hydrogen-bond networks with interfacial water through electron donation, which in turn promotes OH desorption kinetics. Quasi-in-situ XPS and density functional theory calculations further elucidated that the increased electron density on surface OH species reduces OH adsorption energy, thus accelerating HER performance. These findings unveil a direct correlation between surface OH basicity and HER efficiency, offering new insights into tailoring surface environments for advanced water-splitting electrocatalysts.
研究领域:
电化学
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材料科学
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DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Yongsheng Zhang,Hongyong Xue,Mengqing Cheng,Xiaomeng Yang,Zhen Zhang,Xinru Zhao,Armin Rezayan,Dandan Han,Dan Wu,Chunbao Xu
Selective hydrogenolysis of C–O bonds in biomass-derived oxygenated molecules is of great significance for the conversion of biomass to chemicals and fuels, especially for the inert C–O–C bonds in tetrahydrofuran rings. However, the lack of precise active sites results in the low activity of this reaction. In this work, the metal–support interfacial structure of the Ni–La2O3 catalyst was well-controlled by reducing LaNiO3 perovskite at different temperatures. During the reduction, the exsolution and segregation of Ni in the LaNiO3 perovskite led to the formation of metallic Ni nanoparticles and interfacial oxygen-vacant Ni2+-Ov-La3+ sites. Hydrogen spillover from Ni nanoparticles to the interface promoted the in situ generation of La–OH species under reaction conditions. At the same time, the oxygen vacancies at the interfacial Ni2+-Ov-La3+ sites can accommodate the spilled H, inducing the formation of the La–H species. The hydroxyl group in tetrahydrofurfuryl alcohol (THFA) interacted with La–OH through a metal alkoxide intermediate, which was subsequently hydrogenolyzed by the La–H to produce 1,5-pentanediol (1,5-PeD). The intimate La–H and La–OH bifunctional sites on the metal–support interface have a strong synergistic effect, endowing the Ni–La2O3 catalyst with a high THFA hydrogenolysis activity. The proposed interfacial La–H assisted C–O bond hydrogenolysis provides an idea for the design of efficient hydrodeoxygenation catalysts for biomass upgrading.
研究领域:
催化化学
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材料科学
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可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Zhichao Shen,Yanbin Qi,Wangxin Ge,Hongliang Jiang,Chunzhong Li
Urea electrooxidation reaction (UOR) plays an important role in environmental protection and energy regeneration. The extensively studied nickel-based catalysts exhibit good activity for UOR, but urea is more prone to be overelectrooxidized to another pollutant NOx– (x = 2, 3). Herein, the Cu/Ni-B interface catalyst is presented. The introduction of Cu significantly enhances the Faradaic efficiency of N2 (nearly 70% at 1.70 V versus RHE). Electrochemical tests and in situ Raman spectroscopy results show that the introduction of Cu significantly affects the density of OH* species on the catalyst in the UOR process. It is proposed that with a moderate decrease in OH* density, the catalyst can provide enough sites for urea molecules to allow simultaneous adsorption of the two N atoms, facilitating the process of N-N coupling to form N2. This work is also instructive for the design of electrocatalysts for other nucleophile electrooxidation reactions.
研究领域:
电化学
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催化
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环境科学
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能源转换
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
·
IF 15.7
Yanbin Qi,Yihua Zhu,Hongliang Jiang,Chunzhong Li
Designing efficient, stable, and easily scaled-up catalysts for nucleophile oxidation reactions (NOR) is a key step in promoting the industrial application of NOR. Here, a simple physical mixing strategy is adopted to prepare a mixture of NiMo oxide and CoMo oxide as catalyst for methanol electrocatalytic oxidation reaction (MOR). The mixture exhibits high catalytic activity for MOR and its performance far exceeds that of a single component. The interaction at the contact interface between nickel and cobalt components is clarified through operando electrochemical impedance spectroscopy, in-situ Raman spectroscopy, and a series of electrochemical tests. The interfacial interaction enhances the charge transport and promotes the formation of electrophilic OH* species, which significantly boosts the methanol oxidation reaction. This work provides a new idea for the design of efficient and easily scaled-up catalysts for nucleophile oxidation reactions.
研究领域:
催化
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电化学
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材料科学
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可持续能源
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）