INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Jing He,Guangyu Jia,Peiwen Wu,Yingcheng Wu,Hongping Li,Linjie Lu,Zhendong Yu,ShuaiShuai Zhou,Wenshuai Zhu,Huaming Li
Recently, production of a clean sulfur-free fuel and related green chemical processes have attracted the attention of researchers. The development of efficient desulfurizers is an effective strategy to meet this demand. Herein, a facile method to successfully construct W18O49 nanoneedles (NNs) coupled with Pt species by a spontaneous redox reaction between reductive supports and oxidative platinum precursors was revealed. The closely arranged NNs hybrids with strong metal–support electron interaction and in situ-derived carbon are successfully constructed. The Pt species are stabilized on the defective W18O49 NNs surface, which accelerates the adsorption and activation of molecular oxygen. The monolithic catalyst promotes the oxidation conversion of dibenzothiophene in the process of catalytic reactive-type desulfurization. By adjusting the reaction conditions, the catalyst shows over 99.0% dibenzothiophene conversion at only 0.8% Pt loading, and the polar products can be completely removed by extraction. Also, the catalyst showed a relatively stable regeneration and reused performance.
研究领域:
材料科学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jingyi Wang,Guangzhi He,Chunying Wang,Xudong Chen,Xiaofeng Liu,Yaobin Li,Wenpo Shan,Hong He
Modulating the electronic metal-support interaction (EMSI) is one of the effective means to promote catalytic activity because it can adjust the electron occupancy of the d -band of noble metals, further facilitating the activation of reactants. Herein, we prepared a Pt/SiO 2 catalyst with an ultralow Pt loading of 0.05% and found that its catalytic activity in HCHO oxidation outperformed that of the Pt/TiO 2 counterpart, owing to the EMSI effect between Pt and SiO 2 . On this basis, the alkali metal Na was used as a promoter, and the formation of highly active Pt-O x (OH)-Na clusters enabled the complete oxidation of HCHO at room temperature. With ultralow Pt loading, the Pt-Na/SiO 2 catalyst reduces the cost of practical application remarkably. In situ DRIFTS and DFT calculations confirmed that the reaction pathways were distinct on Pt/SiO 2 and Pt-Na/SiO 2 . Specifically, on Pt-Na/SiO 2 , the reaction follows the mechanism of the direct degradation of formate species with the assistance of active hydroxyls; while on Pt/SiO 2 , CO is the only intermediate formed by the dehydrogenation of HCHO, due to the lack of active hydroxyls. These findings provide new insights into the reaction pathway of HCHO oxidation.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 71
·41561-41568
·
IF 3.049
Cuifeng Jiang,Xiaoxiu Wei,Shuai Bao,Huajian Tu,Wei Wang
Nanomaterial-based artificial peroxidase has attracted extensive interests due to their distinct advantages over natural counterpart. Cu@Au/Pt and Cu@Ag/Pt nanocomposite with rambutan-like structure were prepared and discovered to function like peroxidase, which was illustrated by catalyzing the oxidation reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) accompanied with a blue color change. Steady-state investigation indicates that the catalytic kinetics of Cu@Au/Pt and Cu@Ag/Pt all followed typical Michaelis–Menten behaviors and Cu@Au/Pt showed a strong affinity for H2O2, while Cu@Ag/Pt showed strong affinity for TMB. The color change and absorbance intensity strongly depend on the concentration of H2O2, thus the direct determination of H2O2 and indirect detection of glucose were demonstrated using Cu@Au/Pt with a detection limit of 1.5 μM and 6 μM, respectively. What is more important, the method was applied for detection of glucose in 50% fetal bovine serum with a detection limit of 80 μM, which is much lower than the lowest glucose content in blood for diabetes (7 mM). Moreover, the Cu@Au/Pt nanocomposite were also successfully applied for sensing L-cysteine because of the inhibition effect. Considering the good peroxidase-like activity and novel structure, Cu@Au(Ag)/Pt is expected to have a wide range of applications in bioassays and biocatalysis.
研究领域:
生物化学
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纳米医学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2022
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IF 8.047
Hao Zhang,Qiuye Li,Bowen Li,Bo Weng,Zhihong Tian,Jianjun Yang,Johan Hofkens,Feili Lai,Tianxi Liu
We report a porous metal–organic framework loaded with single Pt atoms, namely PCN-222(Pt) nanorods, which are prepared by the self-assembly of Pt-metalized tetrakis(4-carboxyphenyl)porphyrin ligand with a Zr 6 cluster. The mass-loading of Pt in the synthesized PCN-222(Pt) is up to 4.67%, and can be accurately controlled by using an in-situ reaction strategy. Remarkably, the PCN-222(Pt) exhibits a highly efficient photocatalytic hydrogen production rate of 614 μmol g -1 h −1 , which is 7.4 times higher than that of PCN-222 (an isostructural sample to PCN-222(Pt) without coordinated Pt ions in the porphyrin rings). The apparent quantum efficiency of PCN-222(Pt) reaches up to 1.049% at 420 nm. Electron paramagnetic resonance spectra confirm the as-formed intermediate Zr III , obtained from the reduction of Zr IV species, participates in the photocatalytic reaction. Density functional theory calculations demonstrate the positive role that single Pt atoms in PCN-222(Pt) play in optimizing the corresponding hydrogen binding energy. The existence of this dual reaction mechanism in PCN-222(Pt) greatly and synergistically boosts the photocatalytic H 2 production activity.
研究领域:
材料科学
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催化
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光催化
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能量转换
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Hongyu Dong,Panpan Tang,Xinran Wang,Ke Li,Yiwen Wang,Dong Wang,Hui Liu,Shuting Yang,Chuan Wu
Developing efficient and low-cost multifunctional electrocatalysts is important for electrochemical devices. In this work, a cost-effective Pt/NiO composite with very limited Pt loading (from 0.5 to 3%) was controllably synthesized through facile hydrothermal procedures. The composite demonstrated the improved catalytic performance as applied to the nonaqueous Li–O2 batteries and the alkaline fuel cells. Regarding the alkaline fuel cells, 1% Pt/NiO composite gave rise to the best Pt distribution and thus exhibited the optimized electrochemical conductivity and properties as suggested by the significantly improved electrochemical reversibility. Meanwhile, the demonstrated 1% Pt/NiO composite presented high catalytic capability as electrode for Li–O2 batteries, which allowed for much improved capacity utilization, high cycling stability, high initial capacity (2329 mAh/g), and no obvious voltage drop during cycling. Such multiple advantages of prepared composite electrode material offer new prospects and application as multifunctional electrocatalysts for both Li–O2 batteries and alkaline fuel cells.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Jingyi Ma,Hui Yuan,Changcheng Liu,Jieguang Wang,Rongxin Zhang,Aizeng Ma
Propane dehydrogenation (PDH) is used to increase propylene production and to produce hydrogen as a by-product. Despite the widespread utilisation of Pt-loaded catalysts in industrial PDH operations, challenges such as excessive noble metal loading and coking persist in the face of rigorous reaction conditions. These hindrances limit to achieving the optimal economic efficiency. In this work, we report a method aimed at reducing Pt loading to only 0.05 wt% through synergistic modification of GaPt catalysts loaded on SiO 2 -Al 2 O 3 supports (i.e. SIRAL) with K and Ce. The resulting catalysts exhibit remarkable stability and elevated activity for propane dehydrogenation. The K + and SiO 2 could modulate the support surface acidity and immobilizes the active tetrahedral Ga 3+ sites, which improves the catalytic performance and reduce coke deposition. Furthermore, the inclusion of Ce decreases the electron density of the Pt species, stabilizing the atomically dispersed Pt and enhances the formation of active Pt sites, which effectively impedes the Pt agglomeration. As a result, the GaPtKCe/SIRAL10 catalyst demonstrates excellent catalytic performance, achieving 47% propane conversion and >96% propylene selectivity, while maintaining notable stability with 0.016 h −1 deactivation rate constant at 580 °C, even without hydrogen co-feed.
研究领域:
化学工程
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催化材料科学
✓ 已验证
DOI
高影响因子
CATALYSIS SURVEYS FROM ASIA
·
2025
·
IF 2.3
Zhu Mengxuan,Li Hongqing,Wang Xin,Wang Longyang,Wang Rui,Jiang Heng,Jin Changzi
Design of efficient metal-acid bifunction catalysts is of significance for development of hydroisomerization of linear alkanes. In this study, the spatial configurational construction of Pt-ZSM-5 catalytic system was achieved by fabrication of acidic ZSM-5 zeolite and mesoporous silica core-shell composites equipped with controlled location of Pt sites, which aim to explore the effect of functional sites proximity on isomerization reactivity. A series of characterization techniques such as X-ray diffraction, transmission electronic microscopy, N 2 physical adsorption, NH 3 temperature programmed desorption, X-ray photoelectron spectroscopy and so on had confirmed that the synthesized core-shell bifunctional catalysts with different Pt location possessing similar textural, acid and metal properties. In the catalytic hydroisomerization of n -heptane, however, the catalyst with Pt sites locating at acid zeolite exhibits superior n -heptane conversion and isomerization selectivity, which indicates that proximity of active sites at atomic scale may be more conducive to their synergistic effect when the diffusional limitation from zeolitic channel is minimized. These results had presented new direction for the preparation of efficient bifunctional catalysts in hydroisomerization of linear alkanes.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Mengya Guo,Feng Wang,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Encapsulation of clean metal nanoparticles (NPs) into interior of metal–organic framework (MOF) is of great importance to remarkably improve the stability and tune the catalytic performance of metal NPs. Herein, highly dispersed Pt NPs are encapsulated in UiO-66 with different functional groups on linker (UiO-66-X, X = F, H, NH 2 , OH) through enhanced electron attraction of metal precursor by MOF node and proper reduction by H 2 /Ar gas. Compared with traditional impregnation method, the encapsulation method gives well-defined Pt NPs and controllable microenvironment. Detailed characterizations reveal that functional group of the linker can effectively tune the microenvironment and electronic properties of guest Pt NPs. In situ FTIR was utilized to investigate the adsorption capability and strength of reactants on the catalysts. The electron-deficient Pt species and appropriate surface hydrophobicity match well with the reactants, which is responsible for enhanced catalytic hydrogenation activity of C C and nitro groups. The surface hydrophobicity plays a major role in promoting alkyne hydrogenation. This work is devoted to rationalize the relationship between hydrogenation performance and catalyst property of UiO-66 encapsulated Pt NPs, in terms of energy adaptability in electronic state and structure adaptability in surface chemistry. Rational design strategy of Pt-confined-in-MOF composites through molecular level regulation is provided for hydrogenation.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 19
·6879
·
IF 4.6
Tiantian Zhang,Jiacheng Xu,Yan Sun,Shiyu Fang,Zuliang Wu,Erhao Gao,Jiali Zhu,Wei Wang,Shuiliang Yao,Jing Li
Pt-based catalysts exhibit unique catalytic properties in many chemical reactions. In particular, metal–support interactions (MSI) greatly improve catalytic activity. However, the current MSI mechanism between platinum (Pt) and the support is not clear enough. In this paper, the interaction of 1 wt% Pt nanoparticles (NPs) onβ-MnO2in carbon monoxide (CO) oxidation was studied. The Pt onβ-MnO2inhibited CO oxidation below 210 °C but promoted it above 210 °C. A Pt/β-MnO2catalyst contains more Pt4+and less Pt2+. The results of operando DRIFTS-MS show that surface-terminal-type oxygen (M=O) plays an important role in CO oxidation. When the temperature was below 210 °C, Mn=O consumption on Pt/β-MnO2was less thanβ-MnO2due to Pt4+inhibition on CO oxidation. When the temperature was above 210 °C, Pt4+was reduced to Pt2+, and Mn=O consumption due to CO oxidation was greater thanβ-MnO2. The interaction of Pt andβ-MnO2is proposed.Keywords:metal–support interaction;CO oxidation;terminal-type oxygen;bridge-type oxygen;Pt;MnO2
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Shushu Huang,Dengyao Yang,Qianxi Tang,Wei Deng,Long Zhang,Ziye Jia,Zhengfang Tian,Qiang Gao,Limin Guo
In this study, the Pt-loaded ellipsoidal nanozeolite (Pt/ZSM-5-OS) was successfully synthesized by the mercaptosilane modification assisted Pt dispersion method and investigated for the catalytic combustion of toluene, which was used as a model compound of volatile organic compounds (VOCs). The catalytic activity evaluation showed that Pt/ZSM-5-OS exhibited an excellent activity in toluene catalytic combustion, with 90% conversion (T 90 ) occurring at just 164 °C. The catalytic activity was much higher than the catalyst prepared by traditional impregnation method (Pt/ZSM-5-IM, T 90 = 196 °C). In addition, the excellent properties of anti-water vapor and catalytic stability were observed for Pt/ZEM-5-OS. The as-prepared catalysts were characterized by X-ray diffraction (XRD), N 2 physisorption , scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Characterization of the as-prepared catalysts demonstrated that the enhanced catalytic performance was related to the improved Pt dispersion and higher Pt 0 proportion of Pt-ZSM-5-OS. Hence, Pt/ZSM-5-OS and its preparation method are attractive for the practical VOCs catalytic combustion.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Jinxu Xi,Qineng Xia,Yi Shao,Daqian Ding,Panpan Yang,Xiaohui Liu,Guanzhong Lu,Yanqin Wang
Liquid bio-fuels derived from renewable biomass are of great importance on the potential substitution for the diminishing fossil fuels. Aqueous-phase process of sugar and sugar-derived molecules can be used to produce a range of alkanes and oxygenates. In this work, Pt/NbOPO 4 multifunctional catalyst was used in the alkane production by the hydrodeoxygenation of sorbitol in aqueous solution. The results indicated that Pt/NbOPO 4 catalyst showed the highest activity with 60% yield of C6 and C5 alkanes at 250 °C and 4 MPa H 2 among a series of catalysts. The reaction pathway showed that this process included dehydration, hydrogenolysis and CC bond cleavage. Isosorbide is the product of dehydration reaction and also an important intermediate in this process, which undergoes ring opening and following hydrogenolysis to form C6 hexane. The activation energy of sorbitol dehydration and isosorbide hydrogenolysis was calculated, that is 72.7 kJ/mol and 147.6 kJ/mol, respectively, over Pt/NbOPO 4 catalyst, much lower than those over Pt/ZrP and Pt/H-Beta catalysts, which would be attributed to the strong and high acid amount of NbOPO 4 as well as the promotion effect of NbO x for CO bond cleavage. The above results also showed that isosorbide hydrogenolysis is the rate-determine step. More importantly, Pt/NbOPO 4 catalyst was very stable, there was nearly no decrease of sorbitol conversion and no change of products distribution after working in a fixed bed reactor for 100 h. Therefore, Pt/NbOPO 4 is an efficient and stable catalyst for hexane production from sorbitol in aqueous media.
研究领域:
能源科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ruiqi Guo,Zhenglong Fan,Qiwei Zhou,Mengjie Ma,Wenxiang Zhu,Fan Liao,Hao Yang,Jiajie Wang,Zhenhui Kang,Minqi Sheng
Iridium oxide (IrO 2 ) has traditionally been considered to exhibit limited oxygen-reducing capacity. An effective approach to improve the oxygen reduction reaction (ORR) activity in parent catalytic materials is through atomic intercalation. However, the challenge lies in achieving a delicate balance between high ORR activity, structural stability, and minimizing the use of precious metals. Herein, we fabricate 3R-phase iridium oxide (3R-IrO 2 ) with superior ORR activity by intercalating a tiny amount of Pt (3.6 wt% Pt) into the interlayers of 3R-IrO 2 (3.6 wt% Pt-3R-IrO 2 ). When employed as an acidic ORR electrocatalyst, 3.6 wt% Pt-3R-IrO 2 shows a high half-wave potential (E 1/2 ) of 0.92 V (vs. RHE) in O 2 -saturated 0.1 M HClO 4 electrolyte, much better than those of Pt/C (0.850 V), 3R-IrO 2 (0.616 V), and Pt nanoparticles on 3R-IrO 2 surface (3.6 wt% Pt@3R-IrO 2 ) (0.618 V) electrocatalysts. It achieves high mass activity of 0.170 A mg Ir −1 at the potential of 0.9 V, which is 5.5 and 11.3 times than that of Pt/C (0.031 A mg Ir −1 ) and 3.6 wt% Pt@3R-IrO 2 (0.015 A mg Ir −1 ), respectively. Density functional theory (DFT) calculations and experiment results co-jointly demonstrate that the active center of Pt-3R-IrO 2 is anchored to the activated Ir atoms of the 3R-IrO 2 rather than Pt atoms. The d -band center of Ir 5 d orbitals of Pt-3R-IrO 2 is simultaneously regulated, which optimizes the energy barrier of adsorption/desorption toward the ORR process. Intriguingly, the intercalation of Pt atoms into trigonal rhodium oxide (Tri-RhO 2 ) also activates the ORR activity of Rh, suggesting the universality of this strategy. This discovery may provide a new and general way for activation of ORR activity of other precious metal-intercalated nonprecious metal oxide electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 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）