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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Analytical Methods
·
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
Catalysts
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2022
·Vol. 12
·期 5
·480
·
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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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiapei Wang,Yunfeng Guan,Qin Zhang,Hui Zhu,Xuanke Li,Yanjun Li,Zhijun Dong,Guanming Yuan,Ye Cong
Developing homogeneous dispersion and efficient loading Pt-based electrocalalyst remains a huge challenge for hydrogen evolution reaction (HER). Herein, a facile approach to deposit Pt nanoparticles on two-dimensional V 2 C MXene (Pt/V 2 CT x ) is achieved. Pt nanoparticles with narrow size distribution (∼3 nm) and high loading capacity are uniformly anchored on the surface of V 2 CT x . The obtained catalysts possess outstanding activity and stability for HER. In 0.5 M H 2 SO 4 , the overpotential of Pt/V 2 CT x (20%) is 67 mV, and the Tafel slope is 20.6 mV/dec. The oxygen-rich surface of V 2 CT x can provide good hydrophilicity, low hydrogen adsorption free energy and oxophilicity to provide abundant bonding sites for Pt nanoparticles. Moreover, the intrinsically excellent conductivity of V 2 CT x and strong coupling between V 2 CT x and Pt are also of benefit for improving the charge transfer and accelerating the HER kinetics. Therefore, Pt/V 2 CT x may be a promising candidate for HER.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jun Li,Jinlong Liu,Chen Chen,Jiangnan Guo,Ran Bi,Sheng Chen,Lei Zhang,Min Zhu
Developing effective electrocatalysts with reduced Pt content for fast hydrogen evolution reaction (HER) kinetics toward efficient and stable hydrogen production in alkaline media is highly desirable but rather challenging. Herein, Pt nanoclusters (∼1.6 nm) uniformly anchored on ordered macroporous nitrogen-doped carbon support (Pt-30/NCM) with only 3.39 wt% Pt loading is rationally constructed via a polystyrene spheres (PS) template method followed by an impregnating method as a highly enhanced electrocatalyst for alkaline HER. Benefiting from the enhanced mass and charge transport via the ordered macroporous carbon structure as well as the strong metal-support interaction between Pt nanoclusters and nitrogen-doped carbon framework, Pt-30/NCM exhibits superior intrinsic activity and operation stability compared to the solid counterpart without ordered macropores (Pt-30/NCS), even affording a more than 10 times higher mass activity and much better operation stability after 3000 cycles than those of commercial 20 wt% Pt/C. The density functional theory (DFT) calculations reveal that the strong coupling between Pt nanoclusters and nitrogen-doped carbon support can induce favorable charge transfer for accelerated water dissociation as well as desirable d-band center position for suitable adsorption and desorption of alkaline HER intermediates, thus contributing to remarkably improved kinetics of hydrogen production.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
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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CHEMICAL ENGINEERING SCIENCE
·
2022
·
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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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shaodi Sun,Xiaomin Wu,Zhiwei Huang,Huazheng Shen,Huawang Zhao,Guohua Jing
The strong metal-support interaction (SMSI) has received wide attention in heterogeneous catalysis for the room-temperature oxidation of formaldehyde. An interaction between Pt nanoclusters and oxygen vacancy defects will lead to SMSI over the Pt-based catalysts. In this study, defective two-dimensional (2D) TiO 2 nanosheets were synthesized and successfully anchored Pt nanoclusters with a size of 1.3 nm (0.1Pt/TiO 2 -NS). The 0.1Pt/TiO 2 -NS catalyst displayed a superior activity of > 95% HCHO conversion at room temperature, which was ∼ 50% higher than that obtained for a counterpart having the commercial TiO 2 (Degussa P25) support. The abundant oxygen vacancies and stable Pt nanoclusters on 0.1Pt/TiO 2 -NS by introducing SMSI boosted the excellent activity and stability of HCHO oxidation. By exploring electron transfer, suppression of small-molecule adsorption and encapsulation, SMSI was well demonstrated. Furthermore, electron transfer from Pt to TiO 2 -NS led to the electron-deficient Pt surface. The electron-deficient Pt caused by SMSI will enhance the adsorptions of HCHO and H 2 O/O 2 , subsequently improving the catalytic performance. SMSI between Pt nanoclusters and oxygen vacancies endowed the 0.1Pt/TiO 2 -NS catalyst excellent activity and stability to HCHO elimination. In addition, the mechanism for the high HCHO oxidation performance were examined through analysis of in situ HCHO-diffuse reflectance infrared Fourier transform spectra (DRIFTS).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yujing Chen,Jipeng Meng,Di Bai,Chuang Li,Xiao Chen,Changhai Liang
Pt/xFe/ZSM-23 catalysts with various Fe contents were prepared to explore the influence of extra-framework Fe (EF-Fe) on the n-hexadecane (n-C16) hydroisomerization performance. UV–vis and 57Fe Mössbauer spectroscopic results suggest that the Fe species composition was significantly different under various Fe contents, with (HO–Fe(III)–O–Fe(III)–OH) and [Fe(OH)2]+ as the main Fe species at low Fe content (<1.98 wt %), whereas the Fe2O3 clusters/particles as the dominant ones at high Fe content (>1.98 wt %). Moreover, the concentration of Brønsted acid sites and Pt dispersion could be controlled by tailoring the Fe content. Correspondingly, the hydroisomerization performance of n-C16 over Pt/xFe/ZSM-23 catalysts was dramatically changed with various Fe contents. The Pt/1.98Fe/ZSM-23 catalyst with 1.98 wt % EF-Fe content exhibited considerably excellent hydroisomerization performance, and both n-C16 conversion and selectivity to iso-hexadecane (i-C16) could reach over 80 wt % when the reaction temperature was 310 °C.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yu Tan,Siyu Liu,Jiawen Sun,Xiaoke Dong,Yike Wei,Kexin Liang,Shenghan Zhang
Hydrogen is a kind of renewable energy for a friendly environment and can promote carbon emission reduction. The Platinum catalytic electrode is widely applied in hydrogen evolution reaction (HER) of water due to its low overpotential. However, it has affected its commercial application because of its high cost. Therefore, developing heterojunction catalysts with Platinum for HER is an effective way to achieve large-scale hydrogen production . In this work, we present a novel PtNBs/NiNRs heterojunction catalyst via the Pt nanoballs in-situ deposition on Ni nanorods array. The results demonstrate that the PtNBs/NiNRs electrodes have superior catalytic activity for HER in an alkaline condition. The hydrogen overpotential of PtNBs/NiNRs is −61.6 mV (RHE) in the alkaline solution, which is lower than the Pt electrode of −184mV. The Tafel plots and EIS were employed to investigate the mechanism and kinetics of the PtNBs/NiNRs in the alkaline solution. The nanostructures of Ni nanorobs and the Pt nanoballs active sites decrease the charge transfer resistance and increase the charge capacitance for the HER process compared to the Pt electrode. The PtNBs/NiNRs heterojunction catalyst electrodes demonstrate promising applications in HER because of their facile preparation, high efficiency, and low value.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yayun Pu,Lu Jia,Qiang Huang,Xiaosheng Tang,Paramaconi Rodriguez,Limin Huang
Lowering Pt loading in the catalyst while maintaining its superior catalytic efficiency during hydrogen evolution reaction (HER) is essential for the large-scale application of water splitting. The utilization of strong metal-support interaction (SMSI) through morphology engineering has emerged as an effective strategy in fabricating Pt-supported catalysts. However, a simple and explicit routine to realize the rational design of morphology-related SMSI remains challenging. Here we report a protocol for the photochemical deposition of Pt, which benefits from the intrinsic difference in absorption capability of TiO 2 to establish proper Pt + species and charge separation domains on the surface. With a comprehensive investigation of the surface environment through experiments and Density functional theory (DFT) calculations, charge transfer from Pt to Ti, the separation of electron-hole pairs, and the enhanced electron transfer in the TiO 2 matrix were confirmed. It is reported that H 2 O molecules can be spontaneously dissociated by the surface Ti and O, generating OH stabilized by adjacent Ti and Pt. Such adsorbed OH group induces changes in the electron density of Pt, consequently favours the H adsorption and enhances the HER. Benefiting from the preferable electronic state, the annealed Pt@TiO 2 -pH9 (PTO-pH9@A) exhibits an overpotential of 30 mV to reach 10 mA cm−2 geo and a mass activity of 3954 A g-1Pt, which is 17-fold higher than the commercial Pt/C. Our work provides a new strategy for the high-efficient catalyst design by the surface state- regulated SMSI.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zhirong Yang,Yao Shi,Yan Lin,Li Luo,Nan Song,Jianyang Lin,Chong Peng,Baokuan Sui,Jing Zhang,Gang Qian,Xinggui Zhou,Xuezhi Duan
Regulation of pore hierarchy has been an important subject in the design of industrial catalysts. Synthesis of alumina without template/additive often results in poor control of morphologies, porosities, and metal dispersion thereafter. Herein, alumina microrods with a tailored pore hierarchy (Rod2) were fabricated without template/additive by tuning the pore structure of the synthetic precursors, which were used as supports of Pt for n -heptane reforming. Improved toluene selectivity was observed at low space velocities as a result of promoted dehydroisomerization of pentacyclic hydrocarbons, presumably due to a combined effect of the desired pore hierarchy and rod morphology. The Pt/Rod2 also showed better resistance to carbon deposition while maintaining good metal dispersion, as compared to alumina supports with spherical morphology or uncontrolled pore hierarchy. The simulation results revealed that the improved toluene selectivity of Pt/Rod2 is attributed to the proper pore combination of meso -pore1 (6–40 nm) and meso -pore 2 (40–300 nm).
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