Chem Catalysis
·
2023
·
IF 9.4
Zhongliang Huang,Siyuan Hu,Yinan Xu,Jinxin He,Dongren Cai,Kang Sun,Jianchun Jiang,Guowu Zhan
Summary The interfacial sites of metal-support catalysts are crucial for catalytic reactions. Herein, we designed well-defined N-Co 3 O 4 /Pt catalysts with N-tailoring metal-support interfaces to promote catalytic activity toward CO oxidation under humid environments. A series of N-Co 3 O 4 /Pt catalysts were fabricated using ZIF-67 nanocubes as self-sacrificing templates, which showed exceptionally high catalytic activity in low-temperature CO oxidation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study indicates that H 2 O molecules undergo dissociative adsorption to form active –OH species (Co 3+ –OH–Pt). Isotopic labeling technique indicates that H 2 O molecules (or –OH groups) contribute to ∼65% of CO 2 production in CO oxidation. Moreover, the amount of N dopant that stabilized the Co 3+ –OH–Pt species was highly dependent on the H 2 O-soaking conditions of ZIF-67/Pt. Density functional theory (DFT) calculations suggest that the COOH ∗ pathway of CO oxidation over the N-Co 3 O 4 /Pt interface is energetically favorable in humid conditions. In particular, the N doping could stabilize the Co 3+ –OH–Pt interface and simultaneously reduce the energy barrier of CO 2 formation from COOH ∗ intermediates.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Shaobin Li,Jingwei Liang,Xiaoguo Tan,Fengbo Li,Xinming Wang,Lin Ma,Li Zhang,Kun Cheng
Electrochemical water splitting is regarded as a promising technology for production of high purity, high volume hydrogen. It is critical to create robust and highly active electrocatalysts in order to minimize the cost of hydrogen generation and enable large-scale commercial production. In this work, a new 2D MoCu-POMOF, [Cu(4-pyz)] 4 @(PMo 12 O 40 ) (4-pyz = 4-(pyridin-4-yl)benzoic acid) was prepared by a simple hydrothermal method , in which PMo 12 nanocluster was encapsulated into cavity of 2D Cu-MOF. The successful establishment of the model in addition to the goal of uniformly dispersed Mo sources target oxygen-rich PMo 12 nanoclusters can also provide rich Mo source and self-oxidative properties for MoO 2 formation. Cu-MOF provides a special layered structure, which ensures the integrity and stability of the structure and provides a rich C source for pyrolysis and improves the conductivity. Ultralow Pt nanoparticles can reduce free energy of hydrogen evolution , which are embedded in MoO 2 /MoOC with porous structure and high electrochemical active surface area . MoO 2 /MoOC and highly dispersed Pt nanoparticles synergistically promote the HER catalysis. Pt@MoO 2 /MoOC demonstrated the excellent HER activity with a low overpotential of 98.99 mV vs. RHE. This work yielded highly active and high stability molybdenum-based HER electrocatalysis and provides the potential for energy conversion.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Han Sun,Fang Xu,Yongmei Hu,Sui-Jun Liu,Haiping Huang
A series of Pt/Ni-MOF nanocomposites with different atom molar ratio of Pt/Ni were synthesized by the traditional hydrothermal method. Various methods including element mapping, X-ray diffraction (XRD) were employed to characterize the crystal structure and surface morphology of the materials. TEM (Transmission Electron Microscopy) confirms that the Pt nanoparticles are highly dispersed onto the Ni-MOF nanosheet surface, which can provide an abundance of active sites for efficient oxidation of methanol. Electrochemical measurements showed that Catalyst b (the atomic molar ratio of Pt to Ni is 2:1 in the precursor materials) exhibited a higher oxidation current density in MOR and larger electrochemically active surface area (ECSA) than other catalysts with different atomic ratios and commercial Pt/C. Meanwhile, the synthesized catalysts showed long-term activity and good resistance to toxicity.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Long Wu,Wenmin Yin,Xuecai Tan,Pan Wang,Fan Ding,Huan Zhang,Biru Wang,Weiyun Zhang,Heyou Han
It is attractive but remains challenging to develop nanomaterials-based methods to realize the colorimetric detection of ultratrace biological analytes. In this work, an HAuCl 4 -H 2 O 2 system was developed for the visual detection of intracellular hydrogen peroxide (H 2 O 2 ) based on the Au-Pt/SiO 2 sensing platform. Owing to their excellent intrinsic peroxidase-like activity, Au-Pt/SiO 2 nanospheres were introduced to catalyze the decomposition of H 2 O 2 and then directly reduce HAuCl 4 into gold nanoparticles (Au NPs) for the naked-eye detection. The produced Au NPs behaved color variations from light purple to wine red as H 2 O 2 concentration increased. Under the optimal conditions, this strategy showed excellent sensitivity for H 2 O 2 with a detection limit of 0.1 nM by naked-eye readout and 0.1 pM by UV–vis spectrometer (S/N = 3), as well as acceptable selectivity for H 2 O 2 , which could meet the demand for the detection of H 2 O 2 in biological systems. The method was further validated by the determination of H 2 O 2 in HeLa cells with low cellular cytotoxicity. Thus, this strategy would provide simple and sensitive detection of H 2 O 2 in biological systems, revealing the potential application in clinical, biological and environmental researches.
研究领域:
生物分析化学
·
纳米生物学
·
医学检测
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Wang Yaju,Zhou Zhiming,Wang Chao,Zhao Leihong,Xia Qineng
The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) with high added value is attraction but challenging. Pt-WOx-based catalysts have been extensively studied in the selective hydrogenolysis of glycerol. The catalyst support and the physicochemical state of WOx play important roles on this reaction. In this paper, Pt-WOx catalysts supported on TiO2 with different crystal forms were prepared and studied for their catalytic performance in hydrogenolysis of glycerol. It was observed that the catalytic performance of anatase-type (A-type) TiO2-supported catalyst (Pt/W/A-Ti) is much better than that of the rutile-type (R-type) TiO2 catalyst (Pt/W/R-Ti) due to its higher stability. Furthermore, the influence of W loading amount and state were thoroughly investigated for the Pt/W/A-Ti catalysts, and Pt/W/A-TiO2 with 5 wt% loading of WOx achieved the best catalytic performance (100% conversion of glycerol and 41% yield of 1,3-PDO under the optimal reaction conditions), owing to the suitable WOx domains and high dispersion of W species, as evidenced by XRD patterns and TEM images. Mechanism study by in-situ DRIFTS experiments indicated that glycerol was first converted to 3-hydroxypropanal and then converted to 1,3-PDO through subsequent reactions.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Qiangqiang Wu,Hanke Li,Guangxing Yang,Yonghai Cao,Hongjuan Wang,Feng Peng,Hao Yu
A variety of adsorbed intermediates have been extensively assigned during CO 2 hydrogenation on Pt/γ-Al 2 O 3 . However, the surface sites where the surface species reside have not been well resolved, which are extremely important to depict the reaction pathways of CO 2 hydrogenation. In the current work, surface species adsorbed on three regions were distinguished by in situ diffuse-reflectance infrared Fourier transform spectroscopy, i.e., contiguous Pt region of Pt nanoparticle, interfacial Pt int -O-Al int region between Pt nanoparticle and γ-Al 2 O 3 , and surface region of γ-Al 2 O 3 away from Pt nanoparticle. The dynamics of adsorbed H species, carbonyl species, bicarbonates, formate species, and adsorbed CO 2 , were identified at different sites, proving that the reaction occurs at the Pt/γ-Al 2 O 3 interface. We found that only the C-containing species at the Pt perimeter are directly active intermediates for the reaction. Such spatial analysis bridges the gap between the hydrogen activation and CO 2 activation, providing a deep understanding of CO 2 hydrogenation. In addition, the interface structure with oxygen vacancy is important for CO 2 activation, driving the reaction through carboxylate (*HOCO) pathway to form CO at the interface rather than formate (*HCOO) pathway and then be hydrogenated at the Pt surface.
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
·
2023
·
IF 9.9
Jiongting Yin,Cheng Wang,Kewang Zhang,Dongmei Liu,Zhengying Wu,Shinichi Hata,Rui Yu,Yukihide Shiraishi,Yukou Du
Developing highly efficient electrocatalysts based on appropriate heterojunction engineering and electronic structure modification for the oxygen evolution reaction (OER) has been extensively recognized as an effective approach to increase the efficiency of water splitting. Herein, ultralow Pt-loaded (1 %) NiCoFeP@NiCoFe-PBA hollow nanocages with well-defined heterointerfaces and modified electronic environment are successfully fabricated. As expected, the obtained Pt-NiCoFeP@NiCoFe-PBA exhibits outstanding performance with a low overpotential of 255 mV at 10 mA cm −2 and a small Tafel slope of 57.2 mV dec -1 . More specifically, the highly open three-dimensional structure, exquisite interior voids and abundant surface defects endow Pt-NiCoFeP@NiCoFe-PBA nanocages with more electrochemical active sites. Meanwhile, experimental results and mechanism studies also reveal that the construction of heterogeneous interfaces as well as incorporation of noble metals could readily induce strong synergistic effects and significantly tailor electronic configurations to optimize the binding energy of the intermediates, thereby achieving prominent OER performance.
研究领域:
材料科学
·
电催化
·
能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shuang Liu,Nan Zhao,Liyuan Zheng,Richard I. Foster,Wonseok Yang,Zhe Wang,Yuexiang Lu
Photocatalysis has been regarded as one of the effective methods of removing U(VI) from radioactive wastewater in recent years, due to the benefits of being environmentally friendly and efficient. In this work, a Pt cluster modified carbon nitride photocatalyst (Pt-CN) was synthesized in zinc chloride molten salt. The photocatalysts were characterized by XRD, IR, XPS, UV–vis, PL and EIS. The result demonstrated that the doping of Pt makes Pt-CN show higher electronic conductivity and better charge separation and migration, leading to an enhanced photocatalytic activity and faster kinetics compared with bulk graphitic carbon nitride (g-C 3 N 4 ). Moreover, for uranium contained solution photocatalytic treatment, Pt-CN reached 94.6 % removal efficiency after 300 min of illumination with Xe light, and the kinetics improved by a factor of three compared to that of g-C 3 N 4 . Furthermore, the good reusability and photostability of the Pt-CN was confirmed as the removal efficiency remained at 83.7 % even after being recycled and reused five times. The photocatalytic reaction product was characterized as (UO 2 )O 2 ·2 H 2 O, and the mechanism was deduced as uranium species reacting with H 2 O 2 generated by light illumination in an open system. This molten salt one-step synthesis and Pt doping method and the performance of U(VI) extraction in air showed a promising potential for the application of Pt-CN for U(VI) extraction and removal from water.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2016
·Vol. 146
·期 8
·1408-1414
·
IF 2.294
Kang Yumei,Bu Xiaosong,Wang Guangyu,Wang Xiaoqing,Li Qianwen,Feng Yisi
Abstract A series of bimetallic Cu samples (Cu–Pt/SiO 2 , Cu–Pd/SiO 2 , Cu–Ag/SiO 2 , Cu–Ni/SiO 2 ) were prepared by wetness impregnation method, then investigated for hydrogenolysis of glycerol to 1,2-propanediol (1,2-PDO). We furthered the study and found that Cu–Pt/SiO 2 got the smallest particle size and greatest dispersion. Besides, it was found that Pt promoted reduction of Cu 2+ . Compared with other Cu–Pt molar ratio, Cu–Pt/SiO 2 (1:0.2) was the preferable catalyst for hydrogenolysis of glycerol to 1,2-PDO. It is worth noting that Cu–Pt/SiO 2 presented the highest activity with a 96 % selectivity to 1,2-PDO and a nearly 100 % conversion of glycerol at 473 K, 40 bar initial H 2 pressure, 12 h, which is much higher activity than monometallic Cu/SiO 2 , Pt/SiO 2 and other bimetallic Cu samples. Meanwhile, the used Cu–Pt/SiO 2 catalyst still preformed high activity. Furthermore, it was found that the presence of Pt decreased the aggregation of particles during the hydrogenolysis of glycerol. Graphical Abstract
研究领域:
催化化学
·
材料科学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Jianjun Ding,Xuxu Sun,Qi Wang,Dong-sheng Li,Xiangyang Li,Xiaoxiao Li,Lin Chen,Xian Zhang,Xingyou Tian,Kostya (Ken) Ostrikov
Advanced photocatalytic systems are actively pursued to address a large number of pressing issues facing chemical engineering in applications. In the photocatalytic process, high-performance catalysts well beyond the current capacity and cost of platinum-carbon composites are required. In this work, Pt/g-C 3 N 4 composite photocatalysts were synthesized using a low-temperature inductively coupled plasma technique to substantially improve the photocatalytic performance for hydrogen production. After the plasma reduction of H 2 PtCl 6 , ultrafine Pt nanoparticles were uniformly deposited on g-C 3 N 4 . By changing the plasma discharge power, the size of Pt nanoparticles, the composition and electronic structure of Pt and the interaction between Pt and g-C 3 N 4 can be effectively controlled. Moreover, Ar plasma modified the surface structure of g-C 3 N 4 to form new active oxygen-containing groups. The Ar-plasma-treated Pt/g-C 3 N 4 composites showed excellent activity for hydrogen evolution under visible light. When Pt/g-C 3 N 4 composite was plasma-treated at 150 W for 40 min, the achieved hydrogen production rate was 1150.8 μmol/h, which is about 63.2 and 4.6 times higher compared to the pristine g-C 3 N 4 and Pt/g-C 3 N 4 composite prepared by the photodeposition method, respectively. Our results indicate that the low-temperature inductively coupled plasma treatment is an effective and promising tool to fabricate high-performance catalytic materials.
研究领域:
材料科学
·
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Shou-Jiang Han,Xue Wang,Bin Zhang,Hong Yuan,Hai Liu,Yi-Hu Ke
In heterogeneous catalytic reactions, the optimization of surface synergy by adjusting noble metal–support interaction remains a significant challenge. In glycerol oxidation reaction (GOR), introducing oxygen vacancies (Ov) through defect engineering to promote electron transfer, and thus, improve catalytic activity is one of the effective methods. In this work, a series of MZrOx solid solution supports (M = Cu, Mn, Fe, Co, Ni, Zn) were prepared by the co-precipitation method. Then Pt nanoparticles (Pt NPs) were loaded onto the MZrOx support by colloidal-deposition method. The supported Pt/MZrOx catalysts were evaluated for GOR under base-free conditions. The results showed that the Pt/CuZrOx catalyst has optimal catalytic performance. The conversion rate of glycerol and the selectivity of glyceric acid reached 90.5% and 71.4%, respectively. Multi-characterization techniques were employed to analyze the physicochemical properties of the catalysts. It was revealed that the incorporation of a certain amount of M-doping could optimize the abundance of oxygen vacancies, Ptδ+ species, redox properties, and surface acid-basic properties of the supported catalysts, while promoting the formation of strong metal–support interactions (SMSIs), thereby synergistically optimizing the performance of catalysts. These results may offer improved insights and methodologies for the rational design of Pt-based catalysts for GOR under base-free conditions.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 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）