CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qiang Huang,Jiayu Yang,Fei Qi,Wenxia Zhang,Nan Zhang,Zhiyu Liang,Jiaxin Liu,Changqing Tian,Xiaosheng Tang,Daofu Wu,Benjun Huo
Photocatalytic conversion of CO 2 to value-added chemicals and fuels is a green and sustainable approach to solve the problems of CO 2 concentration increment and fossil fuels shortage. Employing photocatalysts with high catalytic activity and selectivity to realize CO 2 conversion has attracted extensive attention. However, the efficiency of photocatalysts is still unsatisfied and the selectivity of products is hard to be regulated, hindering their practical applications in large scale commercial purpose. In this work, for the first time, the Au and Pt was co-deposited on the heterostructure consisted of Cu 2 O quantum dots and ReS 2 nanosheets to achieve high efficiency and controllable selectivity during CO 2 photoreduction. The Au-Pt/Cu 2 O/ReS 2 photocatalysts show superior efficiency of CO 2 reduction than that of Au/Cu 2 O/ReS 2 , Pt/Cu 2 O/ReS 2 , Cu 2 O/ReS 2 , Cu 2 O. Such distinct improvement is attributed to the indirect Z-scheme mechanism and Schottky junction effect. Moreover, the synergetic effect of Au and Pt plays an important role of improving the photocatalytic activity, and the Au1-Pt5/Cu 2 O/ReS 2 exhibits the highest R electron of 516.86 μmol/g during one hour of visible light illumination, which is much larger than many recently reported photocatalysts under comparable condition. Meanwhile, the selectivity of CO and CH 4 is effortlessly tunable from 0 to 100% by modulating Au/Pt metal mass ratio due to the strong CO adsorption on Pt metals and the intensive interaction between Au and Pt atoms at the Au/Pt interface. This controllable selectivity provides admirable strategy to tune the component proportion of the gas products for the subsequent conversion into high value-added chemicals or liquid fuels. Our study proposes novel and deep insights into the design and fabrication of practical photocatalysts with high catalytic activity and controllable selectivity to perform efficient CO 2 photoconversion.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
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IF 4.889
He Han,Anfeng Zhang,Limin Ren,Xiaowa Nie,Min Liu,Yi Liu,Chuan Shi,Hong Yang,Chunshan Song,Xinwen Guo
Shape-selective alkylation of toluene with methanol is one of the most attractive promising synthetic routes to para -xylene. To date, modified ZSM-5 zeolites are considered to be one of the best candidate catalysts for this reaction. Although the para -selectivity could be tuned to approaching 100% by modification of the zeolite and optimization of reaction conditions, at present, there is still a lack of effective means to inhibit the rapid deactivation of the catalysts due to coke formation. In this work, a coke-resistant (Pt + Ni)/ZSM-5 zeolite with excellent stability for shape-selective alkylation of toluene with methanol to para -xylene is developed. The pore structure and acid properties of the zeolite are effectively tuned to ensure high para -selectivity. Meanwhile, the co-existence of Pt and Ni species in this catalyst plays the critical role in inhibiting coke formation, as the two species concurrently impede the formation of olefins, the main coking precursors, via two distinctive mechanisms.
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Catalysts
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2022
·Vol. 12
·期 5
·480
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IF 4.501
Xiuyu Sun,Zhenwei Wang,Wei Yan,Chuangan Zhou
The application potential of Pt/Ti4O7has been reported, but the lack of research on the relationship between Pt loading, MSI, and catalytic activity hinders further development. Micron-sized Ti4O7powders synthesized by a thermal reduction method under an H2atmosphere were used as a support material for Pt-based catalysts. Using a modified polyol method, Pt/Ti4O7-5, Pt/Ti4O7-10, and Pt/Ti4O7-20 with different mass ratios (Pt to Pt/Ti4O7is 0.05, 0.1, 0.2) were successfully synthesized. Uniformly dispersed platinum nanoparticles exhibit disparate morphologies, rod-like for Pt/Ti4O7-5 and approximately spherical for Pt/Ti4O7-10 and Pt/Ti4O7-20. Small-angle deflections and lattice reconstruction induced by strong metal–support interactions were observed in Pt/Ti4O7-5, which indicated the formation of a new phase at the interface. However, lattice distortions and dislocations for higher loading samples imply the existence of weak metal–support interactions. A possible mechanism is proposed to explain the different morphologies and varying metal–support interactions (MSI). With X-ray photoelectron spectroscopy, spectrums of Pt and Ti display apparent shifts in binding energy compared with commercial Pt-C and non-platinized Ti4O7, which can properly explain the changes in absorption ability and oxygen reduction reaction activity, as described in the electrochemical results. The synthetic method, Pt loading, and surface coverage of the support play an important role in the adjustment of MSI, which gives significant guidance for better utilizing MSI to prepare the target catalyst.Keywords:platinum;titanium suboxide;electrocatalyst;SMSI
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Sajjad ul Haq,Muhammad Shuaib Khan,Essossimna Djatoubai,Chung-Li Dong,Penghui Guo,Yu-Cheng Huang,Shaohua Shen
Single atoms (SAs) have drawn significant attention, because of their enormous catalytic activity and high atom-utilization efficiency. Particularly, for H2 evolution, SAs decorated on two-dimensional (2D) nanosheets have great potential, because of the distinctive advantages offered by 2D materials, such as abundant surface-active sites, high specific surface area, and better-photoexcited charge carrier separation. Despite the significant advantages of 2D materials as support, the deposition of SAs on 2D nanosheets is still a great challenge and rarely has been reported. This work reports the facile deposition of Pt-SAs and Pt-SAs/nanoclusters (NCs) on Ca2Nb3O10 and N-doped Ca2Nb3O10–xNx nanosheets, respectively, via a modified photodeposition method. We observe that the presence of a suitable concentration of tetrabutylammonium (TBA+) ions is essential for the successful deposition of Pt-SAs and Pt-SAs/NC via Pt–O bond formation on Ca2Nb3O10 and Ca2Nb3O10–xNx nanosheets, respectively. The findings of aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC HAADF-STEM) validated the successful deposition of Pt-SAs on Ca2Nb3O10 and Pt-SAs/NC on N-doped Ca2Nb3O10–xNx nanosheets, which are further validated via X-ray absorption fine structure (XAFS) spectroscopy. As a result, Ca2Nb3O10-PtSA exhibited excellent H2 production: 280.5 μmol h–1, which is 2.7 and 6.1 times higher, compared to Ca2Nb3O10-PtNP (105.08 μmol h–1) and bare Ca2Nb3O10 (46.05 μmol h–1). Furthermore, N-doped Ca2Nb3O10–xNx-PtSA/NC demonstrated 2.0 and 3.6 times superior H2 evolution, in contrast to Ca2Nb3O10–xNx-PtNP under full-spectrum and visible light irradiation (λ > 420 nm), respectively. Consequently, this work provides a new direction for SAs deposition on exfoliated perovskite nanosheets in the presence of TBA+ ions used during exfoliation, offering a potential strategy that can be applied to a large library of nanosheets synthesized via soft-chemical exfoliation.
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APPLIED CLAY SCIENCE
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2022
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IF 5.907
Xuemin Zhong,Yanfu Wei,Samahe Sadjadi,Dong Liu,Mengyuan Li,Ting Yu,Guanzheng Zhuang,Peng Yuan
Aerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2, 5-furandicarboxylic acid (FDCA) is an important reaction for producing green and sustainable chemicals. Herein, natural clay mineral palygorskite (Pal)-supported bimetallic Pt–Pd catalyst for the oxidation of HMF to FDCA in water without the addition of any bases was developed. The 1Pt 9 Pd 1 /Pal catalyst with Pt/Pd molar ratio of 9/1 exhibited excellent catalytic performance, and 100% HMF conversion and 99% FDCA yield were obtained under optimum reaction conditions after 12 h, which was mainly attributed to the synergy between palygorskite and bimetallic Pt–Pd nanoparticles . Palygorskite used as support realized the immobilization and dispersion of bimetallic nanoparticles, increasing the catalytic activity . The basicity of palygorskite and alloying effects between Pt and Pd facilitated the formation of FDCA by synergistically catalyzing the oxidation of alcohol and aldehyde groups in the reactants and intermediates. Furthermore, this catalyst showed good stability and reusability . The present work provides a highly efficient, cost-effective, and environmentally benign catalyst for the base-free oxidation of HMF to FDCA in practical industrial applications.
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Analytical Methods
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2022
·Vol. 14
·期 25
·2541-2548
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IF 3.532
Lixia Su,Yonghuan Su,Bingqian Liu
A new ratiometric electrochemical strategy for immobilization-free detection of Escherichia coli (E. coli) was constructed by using a capture DNA-polyaniline/copper ferrite nanoparticles/graphene oxide (cDNA-PANI/CuFe2O4/GO) composite as capture probes, which has a high specific surface area and good magnetic properties. Then trigger DNA/Au nanoparticles (tDNA/Au NPs) were used as signal amplification labels, and Pt (IV) and Fe (III) were chosen as the signal probes. In the presence of targets, the sandwich format among cDNA-PANI/CuFe2O4/GO, E. coli and auxiliary DNA (aDNA) was realized by using the aptamer recognition system. Then, the tDNA/Au binding could be anchored on the sandwich format due to the principle of base complementation between unpaired aDNA and tDNA. And the unbounded tDNA of tDNA/Au NPs could bind an amount of Pt (IV). After separation using a magnet, a handful of unbound Pt (IV) which remained in the supernatant reacted with a large number of Fe (III) ions, leading to a markedly increased IFe(III)/IPt(IV) value. Oppositely, the sandwich format could not appear in the absence of targets, and even the tDNA/Au could not be immobilized on it. So, the redox reaction between a large amount of Pt (IV) residue in the supernatant and Fe (III) was significantly successful, causing a low IFe(III)/IPt(IV) value. Under optimal conditions, we found that IFe(III)/IPt(IV) was linearly related to the logarithmic E. coli concentration with a low limit of detection (1.862 × 103 cfu mL−1). This devised ratiometric electrochemical method may develop into a powerful and effective means for the detection of E. coli in real samples, which may also be developed as a universal tool for another microorganism.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zilong Shao,Shunan Zhang,Xiaofang Liu,Hu Luo,Chaojie Huang,Haozhi Zhou,Zhaoxuan Wu,Jiong Li,Hui Wang,Yuhan Sun
Methanol is a suitable raw material for in situ hydrogen generation by steam reforming that enables the safe storage and transportation of hydrogen. Pt-based catalysts have been considered promising and effective for methanol steam reforming but suffer from deactivation by metal sintering. In this study, we developed an efficient K-modified Pt catalyst confined within silicate-1 zeolite with a high activity and unprecedented stability for methanol steam reforming. Owing to the confinement effect, the K-promoted Pt@S-1 catalyst remained stable for more than 50 h. The combination of TPSR-MS and DFT calculations revealed that the Pt-K@S-1 catalyst exhibited a synergistic effect between the Pt 0 and Pt δ+ species. The cleavage of the O–H bond in CH 3 OH was activated over Pt 0 sites to produce HCOOCH 3 , whereas Pt δ+ sites promoted the hydrolysis of HCOOCH 3 to HCOOH and ultimately CO 2 and H 2 , thus suppressing the formation of CO and boosting H 2 production.
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MOLECULES
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2022
·Vol. 27
·期 15
·4673
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IF 4.927
Yanru Liu,Jingyun Mao,Yiwei Huang,Qingrong Qian,Yongjin Luo,Hun Xue,Songwei Yang
The Pt-chitosan-TiO2charge transfer (CT) complex was synthesized via the sol-gel and impregnation method. The synthesized photocatalysts were thoroughly characterized, and their photocatalytic activity were evaluated toward H2production through water reduction under visible-light irradiation. The effect of the preparation conditions of the photocatalysts (the degree of deacetylation of chitosan, addition amount of chitosan, and calcination temperature) on the photocatalytic activity was discussed. The optimal Pt-10%DD75-T200 showed a H2generation rate of 280.4 μmol within 3 h. The remarkable visible-light photocatalytic activity of Pt-chitosan-TiO2was due to the CT complex formation between chitosan and TiO2, which extended the visible-light absorption and induced the ligand-to-metal charge transfer (LMCT). The photocatalytic mechanism of Pt-chitosan-TiO2was also investigated. This paper outlines a new and facile pathway for designing novel visible-light-driven photocatalysts that are based on TiO2modified by polysaccharide biomass wastes that are widely found in nature.Keywords:photocatalyst;TiO2;chitosan;H2evolution;LMCT;visible light
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Ruyi Geng,Huanhuan Jia,Youwei Xie,Dahai Pan,Feng Yu,Binbin Fan
UiO-66 supported metal catalysts have shown high catalytic activity and selectivity to cinnamyl alcohol (COL) in the selective hydrogenation (SHYD) of cinnamaldehyde (CAL), but the roles of missing-linker defects (MLDs) in UiO-66 on the catalytic performance of the UiO-66 supported metal catalysts have less been reported. Here, UiO-66 supports with the different amount of MLDs were used as the supports, and three series of UiO-66 supported Pt (Pt/U) catalysts were prepared by sol-impregnation, wet-impregnation as well as in-situ encapsulation methods, respectively. The influences of the MLDs in UiO-66 on the catalytic properties of the prepared Pt/U catalysts in the SHYD of CAL were investigated. The series of Pt/U-720 catalysts with the more MLDs showed higher CAL conversion and selectivity to COL than the corresponding Pt/U-F catalysts with fewer MLDs. The different preparing methods affect the location and dispersion of Pt species on UiO-66 supports and the metal-support interaction, but the location of the supported Pt species on UiO-66 is the critical factor affecting the catalytic properties of Pt/U catalysts. The presence of the MLDs in UiO-66 is the key to preparing UiO-66 supported Pt catalysts with high SHYD performance.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Fuyuan Sun,Ruifa Su,Yingyu Zhou,Hongfeng Li,Fanchen Meng,Yongqi Luo,Shiming Zhang,Weina Zhang,Baoli Zha,Suoying Zhang,Fengwei Huo
High-loading Pt/C catalysts play an important role in the practical application of metal–air batteries and fuel cells because of their superior activity, high conductivity, and commercial availability. It is well known that high loadings always lead to the agglomeration of Pt nanoparticles, resulting in a loss of catalytic activity and stability; thus, it still remains a challenge to prepare high-loading Pt/C catalysts with high dispersion and small particle sizes. Here, we introduce a surfactant-assisted microwave discharge method to prepare high-loading (>40 wt %) Pt/C electrocatalysts with ultrafine particle sizes (∼3.19 nm) and good dispersion. Benefitting from the high-temperature property and reducibility of carbon-induced-arc, the surfactant and Pt precursors undergo rapid decomposition, reduction, and carbonization, generating the structure of Pt@C on carbon black. The carbon derived from the surfactant can not only inhibit the agglomeration of Pt nanoparticles but also prevent the Pt core from toxication, ensuring high activity and stability of the high-loading Pt/C catalyst. When evaluated in the oxygen reduction reaction, the as-prepared Pt/C catalyst demonstrates a comparable activity and better methanol resistance to commercial Pt/C.
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高影响因子
JOURNAL OF POWER SOURCES
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2022
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IF 9.794
Liang Liu,Baocang Liu,Xuan Xu,Peng Jing,Jun Zhang
The electrochemical oxidation of glycerol is considered as a promising route to generate high value-added products. Rationally tuning the electronic structure of Pt catalysts by supporter and modifier is desirable for promoting the activity and stability of glycerol electrooxidation reaction (GEOR). In this work, we report Pt–Bi hybrid nanoparticles anchored hollow titanium nitride nanowires grew on carbon cloth (Pt 1-x -Bi x /TiN HNWs/CC (0≤ x ≤ 1)) as a self-supported monolithic electrode for efficient GEOR. Contributed by 3D porous nanotube structure, high corrosion resistance and conductivity of TiN, and strong electronic coupling effect of Pt, Bi, and TiN, the optimized Pt 0.95 -Bi 0.05 /TiN HNWs/CC electrode exhibits good catalytic activity and stability for GEOR. It shows a high peak current density of 88.4 mA cm −2 or 306.7 mA mg Pt −1 in 0.05 M glycerol +1.0 M KOH solution. After continuous electrolysis for 8 h in 0.05 M glycerol +1.0 M KOH solution at a constant potential of 0.85 V versus reversible hydrogen electrode (vs. RHE), a high glycerol conversion of 87.0%, a moderate selectivity of 36.6% for glyceric acid , and a good stability were achieved, which is superior to other compared electrodes and most of the reported Pt–Bi catalysts.
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高影响因子
Frontiers in Chemistry
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2022
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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.
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高影响因子
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