APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yaowei Lu,Yongxing Wang,Qinghu Tang,Qiue Cao,Wenhao Fang
The synergistic effect in a bimetallic oxide usually plays a vital role in determining the behavior of supported-metal catalysts. We show the unique synergy in a Sn x Mn 1 O y oxide, which can boost the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid (LA) to γ-valerolactone (GVL). On a series of Pt/Sn x Mn 1 O y catalysts with a similar Pt loading ( ca. 0.44 wt%) and a controlled Pt size ( ca. 2.7 nm), the intrinsic TOF presents a volcano-like dependence on Pt 0 sites and Lewis acidity, which is determined by the variable synergistic effect between MnO y and SnO y . The optimal Pt/Sn 0.8 Mn 1 O y catalyst exhibits a high i TOF of 2709 h −1 and achieves 100% selectivity to GVL at 99% conversion of LA at 120 ℃ and 2 MPa of H 2 . DFT calculations demonstrate that the incorporation of Sn can provide a lower energy barrier for the crucial elementary reactions.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Yaru Wang,Jiaqin He,Xunxun Li,Mengmeng Wang,Yuanbo Zhou,Jun Xiao,Dongyun Chen,Jianmei Lu
MnO2 nanotubes loaded with Pt and Ni–Fe spinel were synthesized using simple hydrothermal and sol–gel techniques. After loading with Ni–Fe spinel, the specific surface area of the material increases 3-fold. This change helped to provide more active sites and facilitated the association between the catalyst and volatile organic compounds (VOCs). X-ray photoelectron spectroscopy determined that the adsorbed oxygen concentrations were all greatly increased after Pt loading, indicating that Pt promoted the adsorption of oxygen and so accelerated the combustion process. The performance of the catalyst after loading with 2 wt % Pt was greatly improved, such that the T90 for benzene decomposition was decreased to 113 °C. In addition, the 2% Pt/2Mn@NFO exhibited excellent low-temperature catalytic activity when reacting with low concentrations of toluene and ethyl acetate. This work therefore demonstrates a viable new approach to the development of Mn-based catalysts for the low temperature catalytic remediation of VOCs.
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Journal of Energy Chemistry
·
2021
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IF 9.676
Yaoxin Wang,Jiandian Wang,Ping Zheng,Changyong Sun,Junyin Luo,Xiaowei Xie
Propane dehydrogenation (PDH) provides an alternative route for producing propylene. Herein, we demonstrates that h-BN is a promising support of Pt-based catalysts for PDH. The Pt catalysts supported on h-BN were prepared by an impregnation method using Pt(NH 3 ) 4 (NO 3 ) 2 as metal precursors. It has been found that the Pt/BN catalyst undergoing calcination and reduction is highly stable in both PDH reaction and coke-burning regeneration, together with low coke deposition and outstanding propylene selectivity (99%). Detailed characterizations reveal that the high coke resistance and high propylene selectivity of the Pt/BN catalyst are derived not only from the absence of acidity on BN support, but also from the calcination-induced and reduction-adjusted strong metal-support interaction (SMSI) between Pt and BN, which causes the partial encapsulation of Pt particles by BO x overlayers. The BO x overlayers can block the low-coordinated Pt sites and constrain Pt particles into smaller ensembles, suppressing side reactions such as cracking and deep dehydrogenation. Moreover, the BO x overlayers can effectively inhibit Pt sintering by the spatial isolation of Pt during periodic reaction-regeneration cycles. In this work, the catalyst support for PDH is expanded to nonoxide BN, and the understanding of SMSI between Pt and BN will provide rational design strategy for BN-based catalysts.
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Small
·
2021
·Vol. 17
·期 36
·2102879
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IF 13.281
Nanzhu Nie,Dan Zhang,Zuochao Wang,Yingnan Qin,Xuejun Zhai,Bo Yang,Jianping Lai,Lei Wang
At present, it is still a great challenge to synthesize refractory Pt-based electrocatalysts with excellent active specific surface area, specific activity, and stability by a simple method. Here, a superfast and solvent-free microwave strategy is reported to synthesize refractory ultrafine (≈3 nm) Pt–lanthanide@Ketjen Black (PtM@KB, M = La, Gd, Tb, Er, Tm, and Yb) alloy with densely packed as efficient hydrogen evolution electrocatalysts in a domestic microwave oven for the first time. The optimized Pt 61 La 39 @KB delivers excellent hydrogen evolution reaction (HER) activity with a low overpotential of 38 mV (10 mA cm −2 ) and a high TOF value of 44.13 s −1 (100 mV) in 0.5 m H 2 SO 4 , and performs well in 1.0 m KOH. This method can also be used to grow catalysts on carbon cloth (CC) directly. PtLa@CC shows an overpotential of 99 mV (1000 mA cm −2 ) in 0.5 m H 2 SO 4 and can maintain activity after 500 h. Theoretical calculations reveal the enhanced stability and activity owing to the higher vacancy formation energy of Pt atoms and the optimized value of Δ G H* . Solvent-free microwave strategy constitutes a significant insight into the development of refractory electrocatalyst with ultrafine size and highly dense, which can also work well at high current densities.
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Green Energy & Environment
·
2021
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IF 8.207
Jiaqin He,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
Improving catalytic performance is a yet still challenge in thermal catalytic oxidation. Herein, uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles were successfully fabricated via a SiO 2 template strategy for the total catalytic degradation of volatile organic compounds at low temperature. The introduction of mesopores into the MnO 2 support induces a large specific surface area and pore size, thus providing numerous accessible active sites and enhanced diffusion properties. Moreover, the addition of a secondary noble metal can adjust the O ads /O latt molar ratios, resulting in high catalytic activity. Among them, the catalyst having a Pt/Pd molar ratio of 7:3 exhibits optimized catalytic activity at a weight hourly space velocity of 36,000 mL g −1 h −1 , reaching 100% toluene oxidation at 175 °C with a lower activation energy (57.0 kJ mol −1 ) than the corresponding monometallic Pt or non-Pt-based catalysts (93.8 kJ mol −1 and 214.2 kJ mol −1 ). Our findings demonstrate that the uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles catalyst is an effective candidate for application in elimination of toluene.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2021
·Vol. 104
·期 12
·6319-6334
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IF 3.784
Limin Zhao,Ruifa Jin,Baofeng Zhang
In this paper, a novel Z-scheme photocatalyst Er 3+ :Yb 0.5 Y 2.5 Al 5 N 0.01 F 0.01 O 11.98 /g-C 3 N 4 –Pt–BiPO 4 was synthesized by sol-hydrothermal and calcination methods. The prepared samples were characterized by XRD, SEM, TEM, EDS mappings, XPS, PL, and DRS. In addition, the optimal hydrothermal conditions for the preparation of BiPO 4 were explored with the azofuchsin solution and ciprofloxacin(CIP) solutions as the target pollutants. At the same time, the best calcination temperature and the best calcination time of the Er 3+ :Yb n Y 3−n Al 5 N x F y O 12−x−y and BiPO 4 were investigated. The results showed that the Z-scheme Er 3+ :Yb 0.5 Y 2.5 Al 5 N 0.01 F 0.01 O 11.98 /g-C 3 N 4 –Pt–BiPO 4 photocatalyst has strong redox ability, wide absorption range of visible light, and excellent separation effect of electron–hole pairs, which can efficiently degrade organic pollutants and antibiotic.
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ANALYTICA CHIMICA ACTA
·
2020
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IF 5.977
Yan Liu,Lianying Zhang,Qinge Li,Han Dai,Ting Xiang,Gangyi Yang,Ling Li
In this work, a colorimetric assay for visfatin detection is described. The mixed valence state Ce-MOF (MVCM) modified by platinum nanoparticles (Pt NPs) is used as a novel catalyst. MVCM exhibits excellent intrinsic peroxidase-like catalytic activity due to the spontaneous recycling of the Ce(III)/Ce(IV) system. Pt NPs serve not only as a carrier of the –NH 2 -modified single strand DNA (S1) but also as a synergistic catalyst of MVCM. The capture probe (S2) attached to the streptavidin-modified magnetic beads (Mag-SA) could combine with the aptamer to form the Mag-SA/S2/aptamer complex. When in the presence of the target visfatin, aptamer specifically combines with the visfatin, which induces the release of Mag-SA/S2 from the Mag-SA/S2/aptamer complex. At this time, the [email protected] /S1 complex connects with the released Mag-SA/S2, which quickly catalyzes the 3,3,3′,3′-tetramethylbenzidine (TMB), leading to a color change. Under optimal conditions, the absorbance increases linearly when the concentration ranges from 1 ng mL −1 to 100 ng mL −1 , and the detection limit is as low as 0.11 ng mL −1 . Furthermore, Mag-SA/S2 can be reused at least five times by using the uracil-DNA glycosylase (UDG) and an external magnetic field. The proposed method shows satisfying reproducibility, stability, specificity, and sensitivity, and it was successfully applied to detect visfatin in spiked human serum samples. Thus, it has great potential for clinical research, detection, and catalytic applications.
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Sustainable Energy & Fuels
·
2020
·Vol. 5
·期 2
·532-539
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IF 5.503
Zhen Zhang,Cheng Jiang,Ping Li,Qi Feng,Zhi liang Zhao,Keguang Yao,Jiantao Fan,Hui Li,Haijiang Wang
Pt single-atom catalysts (SACs) have shown great potential for electrochemical catalysis. However, no systematic study of their bifunctional catalytic activity for the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR) has yet been published. More significantly, the reported catalytic capabilities of Pt SACs have almost been exclusively measured using a rotating disk electrode (RDE) with a three-electrode configuration, which does not accurately reflect the catalysts' performance during operation within single-cell devices. Herein, we demonstrate the immobilization of isolated Pt atoms on a carbon nanosheet support doped with ultrahigh N content (12.1 at%; Pt/NCS) to create a bifunctional HER/HOR catalyst. Compared with commercial Pt/C, the developed Pt/NCS catalyst delivered high utilization as well as excellent mass activity enhancement and stability for both reactions. As a final test, a rigorous catalyst evaluation was conducted in both a proton exchange membrane (PEM) electrolyzer and a PEM fuel cell. As expected, with only half the Pt loading of commercial Pt/C, Pt/NCS-based electrodes in the electrolyzer and the fuel cell still exhibited slightly better performance than those based on Pt/C. This work constitutes a huge step from the academic study of Pt-based SCAs to their industrial application, and it focuses more attention on the harsh evaluation and optimization of SACs within commercial-scale devices.
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LANGMUIR
·
2020
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IF 3.557
Qicheng Zhang,Danyun Xu,Junmei Liang,Qianqian Lin,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
Hydrodeoxygenation (HDO) of bio-oil is a crucial step for improving the bio-fuel quality, but developing highly dispersed Pt-based catalysts with high selectivity for target alkanes remains a great challenge. This study presents a fast surfactant-free method to prepare the MoS2-supported Pt catalyst for HDO. Ultrafine Pt nanoparticles with sizes of <5 nm can be readily grown on chemically exfoliated MoS2 nanosheets (NSs) via the direct microwave-assisted thermal reduction. The obtained Pt NPs/MoS2 composites show excellent catalytic performance in the conversion of palmitic acid, and the best selectivity (also the yield) of hexadecane and pentadecane is 80.56 and 19.43%, respectively.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Hui Huang,Jun Wang,Yafei Xu,Rui Xu,Wuke Li
In this paper, a luminescent and thermo-responsive catalyst based on SiO 2 @Pt@PABI-Tb@PNIPAM was prepared by incorporating Pt nanoparticles , luminescent material and mesoporous silica with thermo-responsive polymer. The obtained catalyst was characterized by IR, TGA, UV–vis, SEM, TEM, X-ray photoelectron spectroscopy and luminescence. The hybrid catalyst exhibits “on-off” green luminescence in solution under UV irradiation, which could be observed by eyes. The catalytic results indicate that the dehydrogenation of ammonia borane (AB) catalyzed by SiO 2 @Pt@PABI-Tb@PNIPAM is thermo-controllable and switchable. The SiO 2 @Pt@PABI-Tb@PNIPAM shows high catalytic activity for the generation of hydrogen at room temperature. However, it exhibits much lower catalytic activity at high temperature. The catalysts exhibit excellent durability because the support and polymer could prevent the aggregation and leaching of Pt nanoparticles during catalysis. The catalytic research offers a new approach to the thermo-controllable application in the generation of hydrogen from AB.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Tao Gan,Yifei Liu,Qian He,Hao Zhang,Xiaohui He,Hongbing Ji
Catalytic conversion of biomass-derived 5-hydroxymethylfurfural (HMF) into high-quality biofuel 2,5-dimethylfuran (DMF) is significant for the utilization of biomass but remains a substantial challenge. Herein, we report a straightforward, eco-friendly, and scalable ball milling method for the synthesis of Co-alloyed Pt (Pt1/Co) single-atom alloy (SAA) catalysts at kilogram levels. The catalysts exhibit superior catalytic performance for the hydrodeoxygenation of HMF to DMF, obtaining 100% HMF conversion and 92.9% selectivity to DMF under 1.0 MPa H2 at 180 °C for 2 h. The reaction pathway is also investigated, which shows that the hydrogenolysis of the C═O bond in HMF to form 2,5-dihydroxymethylfuran is the main route during the hydrodeoxygenation and promoted by the synergistic effect of Pt and Co. Pt1/Co SAA catalysts display excellent stability without aggregation after five successive runs. More inspiringly, our method achieves the mass production of Pt1/Co at the kilogram scale, rendering its potential for practical applications. Moreover, by varying acetylacetonate precursors, we show the general synthesis of different Co-supported noble metal SAA catalysts (M1/Co, M = Pd, Ru, Ir, and Rh). Our findings not only offer a facile and readily scalable synthetic approach of SAA catalysts but also open new avenue to the exploitation of biomass.
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RSC Advances
·
2020
·Vol. 10
·期 41
·24705-24711
·
IF 3.119
Bo-Cai Liu,Shao-Li Chen,Xiao-Yu Ling,Qiao-Xian Li,Chang-Wei Xu,Zi-Li Liu
Spinel oxide NiCo2O4 supported on a three-dimensional hierarchically porous graphene-like carbon (3D HPG) material has been firstly used to enhance the activity of Pt for glycerol electrooxidation. The addition of NiCo2O4 into the Pt/HPG catalyst can significantly improve the catalytic performance for glycerol oxidation. When NiCo2O4 is added to the Pt/HPG catalyst, the onset potential is 25 mV more negative than that on the Pt/HPG catalyst without NiCo2O4. The current density at −0.3 V on the Pt–NiCo2O4 (wt 10 : 1)/HPG electrode is 1.3 times higher than that on the Pt (30 wt%)/HPG electrode. The Pt–NiCo2O4 electrode presented in this work shows great potential as an electrocatalyst for glycerol electrooxidation in an alkaline medium.
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