MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Haoxi Jiang,Zhonghua Liu,Chuanxu Yao,Sheng Wang
The emission of volatile organic compounds (VOCs) causes serious atmospheric environmental problems and catalytic combustion is one of the most promising methods in the treatment of VOCs. In this work, the Pt/Hβ catalyst was fabricated via supercritical fluid deposition (SFD) for the first time and its activity was evaluated for toluene catalytic combustion. The preparation conditions during the SFD process were optimized. Na 2 PtCl 6 was selected as the precursor and 450 °C as the reduction temperature. The catalysts prepared by the SFD and impregnation (IM) were compared. The Pt/Hβ catalyst prepared by SFD had smaller size and higher dispersion and its T90 was 25 °C lower than that prepared by IM, which showed obvious size effect. For the similar activity, the Pt loading on catalyst prepared by SFD is only 50% of that on catalyst prepared by IM, showing obvious reduction effect for noble metal.
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高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Xiuhong Zhang,Dong Wang,Xiao Chen,Longwei Meng,Changhai Liang
The hydrogenation of polycyclic aromatic hydrocarbons (PAHs) over highly efficient and stable catalysts to fine chemicals and intermediates for producing chemical materials is an effective approach to realize the high value-added utilization of coal tar and slurry oil. Herein, two kinds of Al2O3-supported Pt and Rh catalysts are synthesized by strong electrostatic adsorption (SEA) and used to catalyze the hydrogenation of anthracene. Compared with the traditional catalysts synthesized by wet impregnation, the Pt/Al2O3-SEA and Rh/Al2O3-SEA catalysts have smaller active metal particle sizes and higher dispersion, which can expose more active centers, showing higher catalytic activity. Interestingly, anthracene may be preferentially adsorbed on the surface of the Pt/Al2O3 catalyst in a parallel manner but on the surface of the Rh/Al2O3 catalyst in a lateral manner, which leads to the different hydrogenation routes. 9,10-Dihydroanthracene is an initial product for the hydrogenation of anthracene, which is rearranged into tetrahydroanthracene and subsequently hydrogenated to symmetrical octahydroanthracene (sym-OHA) over the Pt/Al2O3 catalyst. The high selectivity to sym-OHA (93%) with the conversion of anthracene near 100% can be achieved in the hydrogenation of anthracene at 240 °C and 7 MPa for 10 h. Additionally, due to the strong anchoring effect, the Pt/Al2O3-SEA catalyst shows high stability for six cycles. This work supplies a new tactic to develop high-performance catalysts for selective hydrogenation of PAHs to important monomers for synthesizing chemical materials.
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DALTON TRANSACTIONS
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2022
·Vol. 51
·期 31
·11693-11702
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IF 4.569
Hongqi Geng,Zhijuan Li,Quan Liu,Qi Yang,Huimin Jia,Qiang Chen,Aiguo Zhou,Weiwei He
Nanozymes show great promise in bioanalysis and therapeutics, which largely rely on high catalytic efficiency and selectivity. Inspired by the interfacial electronic interaction between noble metals and transition metal carbides, Pt nanozymes are modified with Ti3C2 MXene nanosheets to construct Ti3C2/Pt hybrids with synergistically enhanced catalytic activity. Although Ti3C2 does not have oxidase and peroxidase-like activity, it can greatly selectively enhance the peroxidase-like activity of Pt nanozymes. Near-infrared irradiation can further increase specifically the peroxidase-like activity of Ti3C2/Pt. The optimal peroxidase-like activity of Ti3C2/Pt is 6 times higher than Pt in the dark and 7.9 times higher than Pt under illumination. This catalytic enhancement is attributed to the interplay of the strong interfacial electron effect and unique photothermal effect of Ti3C2. Using the superior peroxidase-like activity of Ti3C2/Pt, dual mechanism colorimetric methods based on cascade reaction and inhibitory effect are developed for specific detection of glucose and glutathione with a limit of detection of 1.0 μM and 0.0089 μM, respectively. Our work provides an effective means to improve the catalytic activity and selectivity of nanozymes by introduction of an ideal supporter, which will be of value for the design of efficient nanozymes.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Rui Xu,Jun Wang,Yafei Xu,Zhen Yin,Wuke Li
The ultrafine and highly dispersed bimetallic Pt-Pd nanoparticles are successfully anchored on mesoporous silica nanoparticles (MSN). The MSN@Pt-Pd catalyst exhibits excellent catalytic performance in the hydrogen from ammonia borane (AB). When the MSN@Pt-Pd nanoparticles were grafted with luminescent material and smart thermo-responsive polymer, a smart catalyst could be fabricated. The smart catalyst exhibits the thermo-responsive catalytic performance and switchable luminescence. For example, the composite catalyst displays high catalytic activity in hydrolysis of AB at 25 °C. However, it shows much lower catalytic activity when the temperature increases to 35 °C. The smart catalysts could be potentially applied in the self-protection device of dehydrogenation . When the system of dehydrogenation is under high temperature environment, the smart composite catalyst could automatically restrain the production of H 2 for the purpose of safety.
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TALANTA
·
2022
·
IF 6.556
Xin Wang,Min Zhang,Xiaoxu Pang,Kunlun Huang,Zhiyi Yao,Xiaohong Mei,Nan Cheng
Staphylococcus aureus is a frequent pathogenic bacterium that has a significant detrimental influence on the health of the human body. Therefore, developing a practical and portable detection platform is critical to ensuring food safety. Nanozymes are a kind of engineered nanomaterials with superior enzyme-like activities, providing infinite possibilities for the development of highly sensitive analytical assays. In this study, mesoporous core−shell [email protected] ( [email protected] ) nanozymes were synthesized and then applied as a signal amplifier in Staphylococcus aureus colorimetric immunoassay . At the same time, a careful comparative study of the catalytic performance with natural horseradish peroxidase (HRP), [email protected] nanozymes and their complexes [email protected] (HRP coupling with [email protected] nanozymes) were firstly performed, as well as clever using a colorimeter to achieve portable signal output. [email protected] bioprobes enable remarkable peroxidase-like catalytic activity, resulting in the highest sensitivity with a limit of detection (LOD) improved from 1 × 10 5 to 1 × 10 3 CFU/mL. In all, this work conducted a valuable comparative study and presented an improved strategy for the portable detection of pathogenic bacteria, which was expected to be used in a wide range of applications in food safety regulation and biomedicals arenas.
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PubMed
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 16
·e202200509
·
IF 5.497
Jiefei Li,Zhenyu Li,Zexuan Zheng,Xueqiong Zhang,Hao Zhang,Hang Wei,Haibin Chu
Graphical Biomass conversion : Electro-oxidation of glycerol over the Pt/CNT catalyst suffers from the poor activity, low glyceric acid (GLYA) selectivity, and high cost of the noble metal. The incorporation of CeO 2 into Pt/CNT achieves much enhanced yield of GLYA with even half dosage of Pt. Electrocatalytic oxidation of glycerol is a highly efficient way for upgrading glycerol toward fine chemicals. Currently, electro-oxidation of glycerol into the high value-added C3 products remains a big challenge because of the poor catalytic activity, low selectivity, and high cost of the noble metal catalysts, especially in the alkaline medium. Here, we report that the Pt−CeO 2 /CNT (CNT=carbon nanotubes) catalyst remarkably promotes the conversion (86.5 % vs. 37.6 %) and recycling stability for glycerol electro-oxidation reaction, as compared with Pt/CNT. However, the improved catalytic activity of Pt−CeO 2 /CNT is accompanied by the further oxidation of C3 products including glyceric acid (GLYA). By tuning the product distribution by the ratio of CeO 2 and CNT, applied potential, and the Pt loading amount, the high selectivities of C3 products (95 %) and GLYA (59 %) are achieved together with the high glycerol conversion (86 %), leading to the impressive yields of C3 products (81 %) and GLYA (50 %). The unique contributions of CeO 2 includes not only the enhanced catalytic activity and recycling stability, but also the suppressed further oxidation of GLYA. Moreover, higher yield of GLYA is reached over Pt−CeO 2 /CNT even with half loading of Pt, as compared with Pt/CNT.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Ziyu Xue,Dehong Bai,Yu Li,Qiankun Zhang,Tao shao,Peiqing Guo,Dongxia Zhang,Xibin Zhou
In this work, a simple strategy for the rapid detection of Ag + based on nitrogen, sulfur doped graphene quantum dots (N, S-GQDs) decorated platinum nanoclusters (PtNCs) was proposed for the first time. N, S-GQDs decorated PtNCs (N, S-GQDs@PtNCs) were prepared by a reduction method using ascorbic acid (AA) as reducing agent and N, S-GQDs as a stabilizer and morphology directing reagent, respectively. The N, S-GQDs@PtNCs have an excellent peroxidase activity, which could catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H 2 O 2 to lead to an obvious color change. However, Ag + could be reduced to Ag 0 by N,S-GQDs, and the Ag 0 covered the surface of N, S-GQDs@PtNCs causing its peroxidase activity to decrease. Ag + concentration could be quantified by measuring the maximum absorption signal at 652 nm for oxidized TMB with a wide linear range of 0.5–300.0 nM and a limit of detection (LOD) as low as 0.2 nM. In addition, satisfactory results were obtained for the detection of Ag + in actual water samples. The prepared colorimetric sensor had advantages such as simple operation, cost-effective, fast response, and visualization, and had great potential in detecting toxic Ag + in environmental.
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Catalysts
·
2022
·Vol. 12
·期 7
·775
·
IF 4.501
Yang Liu,Gongda Chen,Jianjun Chen,Hejingying Niu
Metal organic framework (MOF) is a type of porous organic material. In this work, three catalysts loaded with noble metal Pt were prepared by NaBH4reduction method with three different morphologies of Ce–MOF as carriers. Their physicochemical properties were characterized by XRD, Raman, FTIR, N2adsorption, SEM, XPS, and TGA. The catalytic performances of different catalysts were evaluated via toluene oxidation and CO2selectivity. Rod–shaped Pt/MOF–BTC exhibited best catalytic performance compared to Pt/MOF–808 and Pt/UiO–66, its T50and T90were 140 °C and 149 °C, respectively. After deducting the effect of specific surface, Pt/MOF–BTC still had the lowest apparent activation energy (62.8 kJ·mol−1), which is due to the abundant atomic Pt and oxygen vacancy content on its surface. After the reaction, the structure of Pt/MOF–BTC may become amorphous according to XRD results. Furthermore, the presence of amorphous structure had no effect on the catalytic activity of the catalyst. In the stability test of Pt/MOF–BTC to toluene oxidation, both toluene conversion and CO2selectivity remained at 100%, and remained stable for 11 h. Moreover, Pt/MOF–BTC also had better resistance to high weight hourly space velocity (WHSV) or water resistance. The catalyst maintained high catalytic activity for 3 times reusability. This study provides valuable experience for the future work of MOF in the field of VOC catalytic oxidation.Keywords:Ce–MOF;noble metal;oxygen vacancy;catalytic oxidation
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JOURNAL OF RARE EARTHS
·
2022
·
IF 4.632
Luyao Zhang,Fuli Tian,Huan Li,Jiangman Meng,Qi Liu,Xiaoqian Guo,Yun Qiu,Jun Zhang,Changyan Li
A series of non-enzymatic graphene functionalized biosensors was developed via deposition precipitation method for lactic acid (LA) detection, which were characterized by transmission electron microscopy (TEM), Raman spectroscopy , X-ray photoelectron spectroscopy (XPS), gas chromatography-mass spectrometry, liquid chromatography-mass spectrometry, and proton nuclear magnetic resonance ( 1 H NMR). The electrochemical performances of the non-enzymatic biosensors were measured by means of the electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) method. The comprehensive analysis of structures shows that Pt, CeO 2 , and GO components interact with each other. During the storing and releasing oxygen, the valence ratio of Ce 3+ /Ce 4+ and the number of oxygen vacancies in CeO 2 change accordingly, which can be conducive to increasing electronic transmission capacity and finally leads to the improvement of electrocatalytic performance. Among them, the Pt/CeO 2 /GO biosensor containing 0.47 at% platinum exhibits an excellent electrochemical detection performance with high sensitivity of 12.3 µA·L/ (mmol·cm 2 ) and a low limit of detection (LOD) of 5.12 μmol/L in a wide linear range from 10 to 900 μmol/L. In addition, the proposed biosensor possesses a promising anti-interference capability, as well as high stability and good reproducibility, which was assessed by testing the cyclic voltammogram in 0.1 mol/L lactic acid one year later. The underlying mechanism was proposed for electrochemical oxidation of LA to carbon dioxide and acetic acid with the synergistic effect among Pt, CeO 2 , and GO. Furthermore, the results of the standard addition method in real samples (human serum and urine samples) reveal that the lactic acid detection of the non-enzymatic Pt/CeO 2 /GO biosensor is accompanied by high reliability. Thus, it will be a valuable biosensor for in vitro detection of lactic acid level in clinical samples.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jin-Tao Du,Meng Qiao,Yuan Pu,Jie-Xin Wang,Jian-Feng Chen
The reduction of nitroarenes is usually catalyzed by heterogeneous catalysts. In this work, highly stable aqueous dispersions of monodisperse Pt, Pd, and Au nanoparticles stabilized by thermosensitive polymer, poly(N-isopropylacrylamide) (PNIPAM), are conveniently synthesized with the average sizes of 2.3, 3.1, and 2.3 nm, respectively. The modulation of the hydrophilic-hydrophobic nano-environments of the catalysts can be selectively provided by utilizing the temperature-responsive characteristics of PNIPAM. They are effective and thermosensitive pseudohomogeneous catalysts for nitroarenes reduction. The decreasing trend of catalytic activity is as follows: PNIPAM-Au > PNIPAM-Pd > PNIPAM-Pt. The catalytic reduction of nitrobenzene (NB), 4-nitrophenol (4-NP), and o-nitroaniline (o-NA) follow the pseudo-first-order kinetics, and the catalytic rates can be tuned by utilizing their temperature-responsive behavior. PNIPAM-Au nanocatalysts exhibit high turnover frequencies (TOF) up to 84, 12.9, and 40 min −1 for catalytic reduction of NB, 4-NP, and o-NA at 20 °C, respectively, which are one of the highest values ever reported.
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Molecular Catalysis
·
2021
·
IF 5.062
Zhen Song,Jiameng Wang,Xiqing Zhang,Fanji Liu,Lihong Zhang
A series of MgF 2 -modified hydrotalcite-like (HT) derivatives supported Pt-In catalysts PtInHTR-X (X = NH 4 F, NaF and KF, R = reduced catalyst) were prepared by combination of hydrothermal method, alkali-etching and impregnation strategy and applied to direct dehydrogenation of isobutane to isobutene. The catalysts and precursors were characterized by XRD, SEM, TEM, XPS, TG, O 2 -TPO and low temperature N 2 adsorption-desorption isotherms. The formation of MgF 2 phase as dopant to modify the catalyst can influence the pore structure and even the surface acid properties of catalysts. Especially, compared with the three catalysts, PtInHTR-KF catalyst had better stability of isobutene selectivity of over 95% after 9 h reaction, and PtInHTR-NH 4 F and PtInHTR-NaF catalysts exhibited more stable isobutane activity of 60%. One of the reasons for this catalytic performance is that small particles of MgF 2 and unsaturated MgF 2 can provide weak acidic sites which can inhibit coke deposition. And it was found the improved catalytic performance was also related to the appropriate In 3+ /In 0 ratio, well-dispersed Pt species and the excellent anti-sintering ability of catalysts modified MgF 2 .
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Feng Zhang,Dongqing Zhang,Wenqi Liu,Jiyuan Miao,Xiaojin Li
Developing a feasible method to massively fabricate low-cost and efficient oxygen reduction reaction (ORR) catalysts is highly anticipated to the commercialization of fuel cells. In this work, N atoms were doped into inert sp2 configuration to alter the spin and charge distribution in the carbon matrix. The Pt/H2–N–C catalyst was successfully prepared by embedding ultralow Pt nanoparticles on N-based carbon. Results indicated that the protonated N-groups at edge sites efficiently regulated the absorption of the PtCl62– anion and widely limited the migration of Pt species at 1000 °C. The acquired Pt/H2–N–C electrocatalyst exhibited high ORR performance in the acidic electrolyte. The high-temperature proton exchange membrane fuel cell (HT-PEMFC) measurement illustrated that the open-circuit voltage and power density of the Pt/H2–N–C catalyst were higher than those of the commercial 20% Pt/C at 150 °C. This work provided a facile strategy to obtain efficient and low-cost Pt catalysts for ORR and HT-PEMFCs.
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