Small
·
2023
·Vol. 19
·期 24
·2207557
·
IF 13.3
Xin Zhang,Tao Wang,Cui Wang,René Hübner,Alexander Eychmüller,Jinhua Zhan,Bin Cai
Electrochemical upgrading of ethanol to acetic acid provides a promising strategy to couple with the current hydrogen production from water electrolysis. This work reports the design of a series of bimetallic Pt Hg aerogels, where the PtHg aerogel exhibits a 10.5-times higher mass activity than that of commercial Pt/C toward ethanol oxidation. More impressively, the PtHg aerogel demonstrates nearly 100% selectivity toward the production of acetic acid. The operando infrared spectroscopic studies and nuclear magnetic resonance analysis verify the preferable C2 pathway mechanism during the reaction. This work opens an avenue for the electrochemical synthesis of acetic acid via ethanol electrolysis.
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高影响因子
ACS Applied Nano Materials
·
2019
·
IF 0
Bin Qi,Chenchen Wu,Yu Liu,Jun Liu,Haibo Zhang
Self-assembled nanotechnology has been used widely in various well-defined microstructures fabrication. Herein, this synthetic protocol was successfully utilized to in situ or hierarchically prepare magnetic Pt nanocomposites Fe3O4@Pt via a distinguishing two-step process. The distinction of these two pathways is due to the different synthetic processes. In the case of in situ preparation (Path I), it involves a supramolecular self-assembly of boron clusters with γ-CD on Fe3O4 substrate and then followed by in situ formation of Pt nanoparticles (NPs). But in the case of hierarchical preparation (Path II), the first step is preparing Pt NPs colloids reduced by boron clusters Cs2[closo-B12H12], and subsequent step is immobilizing the as-prepared [closo-B12H12]2–-capped Pt NPs on the Fe3O4@γ-CD. The success of these two fabrication strategies lies in the use of trifunctional boron clusters (reductant, stabilizer, and superchaotropic anchor). Both of the as-prepared Fe3O4@Pt nanocomposites showed good catalytic performance in the selective nitro-group reduction of nitroaromatics. A control test further indicated that the in situ prepared Fe3O4@Pt nanocomposites, with smaller size and higher loading of Pt NPs, exhibited a better catalytic performance and recyclability.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Shendan Zhang,Mingjie Yang,Kunyu Liang,Ayse Turak,Bingxue Zhang,Da Meng,Chuanxi Wang,Fengdong Qu,Wenlong Cheng,Minghui Yang
Nanosized Pt-loaded Fe 2 O 3 nanocubes are prepared through, successively, a simple hydrothermal reaction, two-step annealing process and finally reduction with NaBH 4 of H 2 PtCl 4 . The resultant Pt decorated Fe 2 O 3 nanocubes, made up of Fe 2 O 3 nanoplatelets, are hierarchical, hollow and porous, with an average edge length of 200–300 nm. The sensor based on Pt decorated Fe 2 O 3 nanocomposites exhibits higher response (R air /R gas = 25.7) to 100 ppm of acetone gas at lower temperature (139 °C), with a short response-recovery time (3 s/22 s), compared with pure Fe 2 O 3 nanocubes sensor. The Pt-Fe 2 O 3 nanocomposite sensor shows excellent potential to act as a low cost, low temperature sensor for acetone gas, with high acetone selectivity under high humidity conditions and with the interference of other gases. Under various environmental conditions designed to mimic exhaled air, the sensor is able to detect ppb amounts of acetone, with high repeatability and stability, making it suitable for applications such as oral diabetic sensors. The attractive chemical and electronic sensitizations of partially oxidized Pt nanoparticles are responsible for the enhancement of acetone sensing performance. Based on the high acetone selectivity, high stability and fast dynamic response, the Pt enhanced Fe 2 O 3 nanocubes sensor is an exceptionally suitable candidate for a low cost acetone sensor, and the proposed approach provides a route to develop gas sensors that can operate at low temperatures for a wide variety of applications.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Qingui Yang,Na Li,Qiang Li,Shaoqing Chen,Hsing-Lin Wang,Haipeng Yang
Sarcosine is a recently identified biomarker for prostate cancer. However, the rapid detection methods for sarcosine are relatively lack because of the low concentration and the presence of complicated interfering substances in serum or urine. In this manuscript, hollow nanospheres of Fe 3 O 4 was synthesized and used as carrier to disperse Pt (Pt) nanoparticles . In order to achieve excellent electron transfer ability, we use polyaniline to coat Pt–Fe 3 O 4 nanoparticles, and pyrolyze the polyaniline to carbon (C). Thus, hollow magnetic Pt–Fe 3 O 4 @C nanocomposites with good electron transfer ability are formed. The Pt–Fe 3 O 4 @C nanocomposites have high catalytic activity and stability. The nanocomposites were immobilized on glassy carbon electrode (GCE) to construct a nonenzyme hydrogen peroxide (H 2 O 2 ) sensor (Pt–Fe 3 O 4 @C/GCE). We further construct a sensitive sarcosine biosensor by immobilizing sarcosine oxidase (SOx) on the Pt–Fe 3 O 4 @C/GCE. The high catalytic activity and good biocompatibility of Pt–Fe 3 O 4 @C nanocomposites greatly retained the bioactivity of immobilized SOx, and the prepared sarcosine biosensor has good electrocatalytic performance towards sarcosine. It has a linear detection range between 0.5 and 60 μM with a limit of detection (LOD) of 0.43 μM (the signal to noise ratio is 3), and the sensitivity is 3.45 nA μM −1 (48.8 nA μM −1 cm −2 ), which has the potential to be used for rapid screening of prostate cancer.
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高影响因子
ACS Applied Nano Materials
·
2019
·
IF 0
Shuo Li,Jiawei Liu,Guilin Zhu,Heyou Han
Conformal deposition of Pt-dots arrays on polyhedral Pd nanocrystals can enhance Pt catalytic properties and reduce its loading. Herein, a simple method for the fabrication of Pd@Pt core–shell nanodot arrays (Pd@PtNAs) heterostructures via reducing H2PtCl6 and Na2PdCl4 by l-ascorbic acid in an aqueous solution with cetylpyridinium chloride and KBr is reported. The Pt nanodots arrays with a small size (about 3 nm in diameter) were dispersed on the surface of Pd decahedra. Such ultrasmall size Pt dots arrays can effectively increase the proportion of low-coordination Pt atoms. Compared with commercially available Pt/C catalysts, the Pd@PtNAs show obvious improvement in catalytic performance applied to oxygen reduction reaction. The mass activity (0.20 A/mgPt) of the obtained Pd@PtNAs with 36.9 wt % Pt shows 2.2 times relative to Pt/C catalyst (0.09 A/mgPt) for ORR. What’s more, the Pd@PtNAs with 36.9 wt % Pt exhibited highly stable property and mass activity with only 11% loss after 10 000 testing cycle.
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CRYSTENGCOMM
·
2017
·Vol. 19
·期 46
·6964-6971
·
IF 3.474
Aleksei Chalgin,Fenglei Shi,Fan Li,Qian Xiang,Wenlong Chen,Chengyi Song,Peng Tao,Wen Shang,Tao Deng,Jianbo Wu
Elemental composition, dimensionality and morphology are the main factors that influence the catalytic activity and stability of platinum-based and noble metal alloy nanocatalysts. Herein, we present a facile and cost-efficient approach to synthesize ternary alloy Pt–Pd–Ag nanoflowers by co-reduction of the metal precursors in aqueous solutions in a suitable molar ratio, involving hexamethylenetetramine as a structure-directing agent and ascorbic acid as a reducing agent. Both the presence of the aforementioned agents and the interaction between the component metals allow good control over the anisotropic growth of the ternary alloy nanostructure. The as-prepared nanocomposite demonstrates superior electrocatalytic activity towards the oxygen reduction reaction in acidic medium, compared with commercial Pt/C (20 wt%) and Pd/C (10 wt%) catalysts, as well as sufficiently good stability, as demonstrated by the accelerated durability test. The electrocatalytic activity of irregularly shaped nanoparticles of the same elemental composition was also measured, which revealed that the nanoflowers were superior catalysts owing to their specific morphological characteristics. Moreover, the nanoflowers displayed a relatively low electrochemical surface area decay (from 100% to 80.82%) due to their three-dimensional open-framework surface which can limit the aggregation of individual particles.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Liming Zeng,Tianxiang Yuan,Zerui Liu,Yongyang Zhu,Daifeng Wu,Dongxing Wang,Qing Zhou,Renheng Tang
Aiming at the sluggish water dissociation step in alkaline hydrogen evolution reaction (HER), the platinum-nickel alloy material (PtNi 10 /C) featuring unique crystalline/amorphous structure supported on carbon black is deliberately designed and fabricated via a reversely rapid co-precipitation and mild thermal reduction strategy. Electrochemical results show that only 66 mV of overpotential is needed for PtNi 10 /C to drive a current density of 10 mA cm −2 at a lower platinum loading (8.3 μg Pt cm-2 geo), which is much lower than that of other catalysts with a single metal source(S-Ni/C and S-Pt/C) and even the commercial Pt/C catalyst (20 wt%). The target catalyst also exhibits smaller tafel slope value (16.73 mV dec −1 ) and electrochemical impedance value, enabling a fast kinetics rate for water dissociation. Partial crystallization facilitates moderate adsorption of intermediates, while the high-valence Ni(II) and Pt(II) species serve as pivotal driving force for the kinetic dissociation of water. The unique microstructure of PtNi 10 /C shows a remarkable advantage toward HER in alkaline but acidic medium. In addition, other transition metal-based catalysts following the similar protocol are also fabricated and present varying degrees of HER performance. Hence, the facile and rapid co-precipitation/thermal reduction strategy proposed in this study provides some guidelines for designing high-efficiency alkaline HER catalysts.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 44
·27515-27523
·
IF 3.945
Yunxiao Zhang,Pengfei Yan,Yannan Zhou,Qun Xu
Impregnating noble metals in metal–organic frameworks (MOFs) for obtaining effective catalysts for the photocatalytic process is of great significance but remains very challenging. Herein, for the first time, atomically dispersed Pt atoms were successfully impregated inside the MOF UiO-66 with the assistance of supercritical carbon dioxide (SC CO2). Our study demonstrated that the SC CO2-directed strategy makes Pt undergo a stable encapsulation inside UiO-66, realizing a stage for the rapid transfer of photogenerated electrons between the components of the composite, hence dramatically increasing the catalytic effect. Further, theoretical calculations demonstrated the experimental characterization of the unique structure. Moreover, the as-prepared hybrid structure of Pt@UiO-66 composites presented an extremely high photocatalytic efficiency for hydrogen evolution under visible-light irradiation. An unusual H2 production rate of 3871.4 μmol h−1 g−1 could be achieved by Pt@UiO-66 under visible-light irradiation. This was nearly 50 times higher than the H2-evolution rate achieved by pure UiO-66 under the full spectrum.
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高影响因子
Nano Today
·
2022
·
IF 18.962
Zhentao Zhang,Haiqing Zhong,Yi Zhou,Peng Ke,Qi Dai,Yiying Lu,Xincheng Zhong,Qiyao Yang,Yiyi Xia,Xiaoyan Bao,Linjie Wu,Min Han,Jianqing Gao
The deep penetration in response to specific intratumoral conditions holds considerable potential in achieving a more effective therapy. Lactate is mainly produced by exuberant-metabolism tumor cells growing in the deep center of solid tumor, which would form the characteristic of higher-level lactate deep inside tumor in distance with blood vessels. Herein, inspired by the in vitro directional chemotaxis of enzyme-powered nanomotor driven by substrate gradient, a novel lactate oxidase (LOX)-powered Pt Nanoflowers (Pt NFs) was developed to achieve deep intratumoral penetration triggered by the lactate-driving positive chemotaxis that was confirmed both in vitro and in vivo for the first time. Besides, LOX-powered Pt NFs with self-oxygenation could achieve a more thorough effect on hypoxic relief via the cascading catalysis: (1) the orthotopic extra H 2 O 2 production from lactate catalyzed by LOX, and (2) the effective conversion of both extra-supplement and endogenous H 2 O 2 into O 2 catalyzed by Pt NFs, further overcoming the hypoxia-induced radioresistance . Meanwhile, the X-ray radiation deposited inside Pt NFs could improve low-dose radiotherapy effect with increasing ROS level and enhancing nuclear DNA damage. Collectively, this work would provide a blueprint for developing substrate gradient-driving "smart" delivery systems and radiosensitization strategy.
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高影响因子
Catalysts
·
2021
·Vol. 11
·期 10
·1219
·
IF 4.146
Jun Qiao,Tian Wang,Kai Zheng,Enmu Zhou,Chao Shen,Aiquan Jia,Qianfeng Zhang
A novel reusable Fe3O4@NC@Pt heterogeneous catalyst was synthesized by immobilizing platinum on nitrogen-doped carbon magnetic nanostructures. It was characterized by infrared analysis (FT-IR), X-ray diffraction (XRD), transmission electron microscopy (TEM), and vibrating sample magnetometer (VSM). The catalytic efficiency of Fe3O4@NC@Pt was investigated by reduction of nitro aromatic compounds. The catalyst showed good catalytic activity, wide range of substrates, and good chemical selectivity, especially for the substrates of compounds containing halide and carbonyl groups. The magnetically catalyst can readily be reused up to ten cycles without loss of catalytic activity. Moreover, the key pharmaceutical intermediateLorlatinican be facilely achieved through this strategy.Keywords:reusable;magnetic;platinum;selective reduction;nitroarenes
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高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Yang Liu,Wei Guo,Xiaojun Li,Peng Jiang,Ning Zhang,Minghui Liang
The selective hydrogenation of alkynes to alkenes is very important for both industry and scientific investigation, and overhydrogenation of alkynes to alkanes is the biggest problem to be solved. Suppressing the catalytic hydrogenation of alkenes to alkanes and keeping the efficient conversion from alkynes to alkenes at the same time is a viable solution, but the slight difference in structure between alkynes and the corresponding alkenes causes great difficulty in realizing such a target. The Pt/C–Cu bimetallic catalysts are used to catalyze the selective hydrogenation of phenylacetylene (PA) to styrene (ST). High-resolution STEM and EXAFS results show that the prepared Pt/C–Cu catalysts are composed of copper single atoms and Pt nanoparticles. In particular, Pt/C–Cu is a catalyst in which copper single atoms cover the surface of Pt nanoparticles. The experimental results reveal that the selectivity of ST strongly depends on the coverage of Cu single atoms over Pt nanoparticles in Pt/C–Cu, so selective hydrogenation of PA is a structure-sensitive reaction. The selectivity of ST can reach 94.4% at a PA conversion of 100% in the selective hydrogenation of PA over Pt/C–0.5Cu, an optimized Pt–Cu bimetallic catalyst; after selective removal of PA in ST from 100 to 30 ppm over the same catalyst, the yield of ST reaches 99.97%. The chemisorption results of H2 and probe molecule ethene (C2H4) over the Pt–Cu/C catalysts reveal that Cu single atoms covering on the surface of Pt nanoparticles weaken the Pt–H and Pt–C2H4 interactions, so the catalytic hydrogenation of the carbon–carbon double bond over Pt/C–0.5Cu can be tremendously suppressed. The added Cu single atoms over Pt nanoparticles are not poisonous sites because they can also act as the active centers to activate hydrogen and the carbon–carbon double bond.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2021
·Vol. 47
·期 10
·4051-4066
·
IF 2.914
Chen Rong,Yi Guohui,Wu Songshuai,Meng Chuangang
Well-dispersed Au–Pt alloyed bimetallic nanoparticles are synthesized using chlorogenic acid as the only reducing agent and stabilizer to reduce Au/Pt precursors successively has been presented here. The shapes of Au–Pt bimetallic nanoparticles are controlled by changing the sequence of successive reduction: the spherical shape in the sequence of Pt precursor reduced prior to Au precursor, and the flower shape by reversing the sequence. The sizes of Au–Pt bimetallic nanoparticles can be tuned by changing the molar ratios of the precursors to chlorogenic acid, and the average size of Au–Pt bimetallic nanoparticles decreased or increased with an increase in chlorogenic acid concentration in different sequence of successive reduction. Additionally, the high antioxidant activity of Au–Pt bimetallic nanoparticles was verified by in vitro radical scavenging assays. Our results show that chlorogenic acid is an excellent reducing and capping agent for the controlled synthesis and stabilization of Au–Pt bimetallic nanoparticles, which could be extended to reduce other metal precursors for synthesizing bimetallic and trimetallic nanoparticles. These shape-controlled and size-tunable Au–Pt bimetallic nanoparticles by chlorogenic acid will expand their biomedical applications in future. Graphic abstract
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高影响因子
危险品化学品经营许可证（带存储）