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Catalysts · 2020 ·Vol. 10 ·期 10 ·1192 · IF 3.52

Steric Effects of Mesoporous Silica Supported Bimetallic Au-Pt Catalysts on the Selective Aerobic Oxidation of Aromatic Alcohols

Jun Yan,Longlong Shan,Xiaoli Gu,Xingguang Zhang,Junmeng Cai

Three series of catalysts consisting of gold (Au), platinum (Pt), or gold-platinum bimetallic nanoparticles (NPs) with controlled sizes (Au NPs 10 ± 2 nm, Pt NPs 6 ± 2 nm) anchored on hierarchical micro-/meso-/macroporous silica were successfully developed and systematically evaluated for the selective oxidation of aromatic alcohols to their corresponding aldehydes. The catalysts were prepared by the sol-immobilization method using as-made Au NPs and/or Pt NPs colloids; the silica supports were prepared with controlled pore structures and the hierarchical porous structures of catalysts were created by controllable desilication via the alkaline solution of the metal colloids. The catalysts were characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS), and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS), and these results showed no synergistic effect between Au and Pt on boosting the catalytic performance, whereas they demonstrated a clear dependence of catalytic conversions and reaction rates on the structural porosity of Au-Pt bimetallic catalysts. Our findings could potentially inspire peer researchers and scientists to develop designer porous catalysts and processes in the selective organic conversions.Keywords:steric effect;Au-Pt catalysts;alcohol oxidation;hierarchical porous silica

研究领域: 催化化学 · 材料科学
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Small Methods · 2023 ·Vol. 7 ·期 7 ·2300121 · IF 12.4

Atomically Dispersed Pt-Doped Co3O4 Spinel Nanoparticles Embedded in Polyhedron Frames for Robust Propane Oxidation at Low Temperature

Gaoyan Xiong,Chao Feng,Hsiao-Chien Chen,Junxi Li,Fei Jiang,Shu Tao,Yunxia Wang,Yichuan Li,Yuan Pan

This study adopts a facile and effective in situ encapsulation-oxidation strategy for constructing a coupling catalyst composed of atomically dispersed Pt-doped Co 3 O 4 spinel nanoparticles (NPs) embedded in polyhedron frames (PFs) for robust propane total oxidation. Benefiting from the abundant oxygen vacancies and more highly valent active Co 3+ species caused by the doping of Pt atoms as well as the confinement effect, the optimized 0.2Pt-Co 3 O 4 NPs/PFs catalyst exhibits excellent propane catalytic activity with low T 90 (184 °C), superior apparent reaction rate (21.62×10 8 (mol g cat −1 s −1 )), low apparent activation energy ( E a = 17.89 kJ mol −1 ), high turnover frequency ( 811×10 7 (mol g cat −1 s −1 )) as well as good stability. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations indicate that the doping of Pt atoms enhances the oxygen activation ability, and decreases the energy barrier required for C  H bond breaking, thus improving the deep oxidation process of the intermediate species. This study opens up new ideas for constructing coupling catalysts from atomic scale with low cost to enhance the activation of oxygen molecules and the deep oxidation of linear short chain alkanes at low temperature.

CAS / MDL: 67-56-1
研究领域: 化学工程 · 材料科学 · 催化反应
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APPLIED ORGANOMETALLIC CHEMISTRY · 2018 ·Vol. 32 ·期 3 ·e4208 · IF 3.581

Novel synthesis of Fe2O3–Pt ellipsoids coated by double-shelled La2O3 as a catalyst for the reduction of 4-nitrophenol

Yan Gao,Jiasheng Fang,Yiwei Zhang,Chao Zhang,Shuo Zhao,Yuming Zhou,Mengqiu Huang,Xiaoli Sheng

A facile strategy is reported for the fabrication of Pt-loaded core–shell nanocomposite ellipsoids (Fe 2 O 3 -Pt@DSL) consisting of ellipsoidal Fe 2 O 3 cores, double-layered La 2 O 3 shells and deposited Pt nanoparticles (NPs). The formation of the doubled-shelled structure uses Fe 2 O 3 -Pt@mSiO 2 as template sacrificial agent and it involves the re-deposition of silica and self-assembly of metal oxide units. The preparation methods of double-shelled metal oxides avoid repeated coating and etching and could be utilized to fabricate other shaped double-shelled composites. Characterization results indicated that the Fe 2 O 3 -Pt@DSL nanocomposites possessed mesoporous structure and tunable shell thickness. Moreover, due to the formation of Fe 2 O 3 and La 2 O 3 composites, Pt NPs can also be stabilized via deposition on chemically active oxides with a synergistic effect. Therefore, as a catalyst for the reduction of 4-nitrophenol, Fe 2 O 3 -Pt@DSL showed superior catalytic activity and reusability due to structural superiority and enhanced composite synergy. Finally, well-dispersed Pt NPs were encapsulated into the void between the shell layers to construct the Fe 2 O 3 -Pt@DSL-Pt catalyst.

CAS / MDL: 100587-94-8
研究领域: 材料科学 · 催化化学
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Reaction Chemistry & Engineering · 2024 · IF 3.4

Synthesis of glycolic acid by selective oxidation of ethylene glycol over Pt/Sn-Beta in a base-free medium

Yongming Xu,Wenzhao Liu,Bo Xu,Ke Wang,Jinchu Yang,Yueqi Si,Xuebin Zhao,Tingting Zhang,Zhan Zhang,Xueyi Qiao,Tianliang Lu

Glycolic acid finds extensive applications in the production of biodegradable polymers, pharmaceuticals, and fine chemicals. In this study, a Pt catalyst supported on the Sn-Beta zeolite (Pt/Sn-Beta) was developed to achieve the efficient and highly selective catalytic oxidation of ethylene glycol with molecular oxygen to prepare glycolic acid at near-room temperature (30 °C). Characterization results, including XRD, TEM, XPS, FT-IR, and O2-TPD, revealed that the relatively uniform dispersion of Pt particles, the optimal density of Lewis and Brønsted acid sites in the catalyst, and the synergistic interaction between Sn and Pt sites might be key factors contributing to the excellent catalytic performance of the Pt/Sn-Beta catalyst. By optimizing the reaction conditions, a 90% conversion of ethylene glycol and an 81% selectivity of glycolic acid were obtained. Furthermore, Pt/Sn-Beta exhibited excellent stability, with no significant decrease in catalytic performance after six repeated uses.

研究领域: 化学工程 · 催化科学
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Construction of two dimensional Sr2Ta2O7/S-doped g-C3N4 nanocomposites with Pt cocatalyst for enhanced visible light photocatalytic performance

Weixuan Zeng,Yuan Bian,Sheng Cao,Anquan Zhu,Lulu Qiao,Yongjin Ma,Pengfei Tan,Quanyin Ma,Rui Dong,Jun Pan

Visible light-driven photocatalytic hydrogen production has been deemed a potential means to solve the increasingly serious energy shortage problem. Herein, two dimensional (2D) Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposites that applied in photocatalytic water reduction were fabricated through thermal condensation of thiourea with hydrothermal-prepared Sr 2 Ta 2 O 7 . The resulted Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposite exhibited enhanced hydrogen evolution rate (11.36 μmol g −1  h −1 ) under visible light irradiation, which is about 3.5 times higher than that of pure S-doped g-C 3 N 4 . In light of the UV–vis diffuse reflectance spectroscopy, Mott-Schottky curve and photoluminescence spectra, the enhanced photocatalytic performance could be mainly attributed to the conduction band difference between Sr 2 Ta 2 O 7 and S-doped g-C 3 N 4 . In addition, transient photoluminescence spectra, electrochemical impedance spectra and photocurrent responses proved that the presence of Pt cocatalyst also plays an important role in facilitates the transport of photoexcited electron-hole pairs, subsequently promoting the photocatalytic performance.

研究领域: 材料科学 · 能源科学
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ACS Applied Nano Materials · 2021 · IF 5.097

Pt and ZnFe2O4 Nanoparticles Immobilized on Carbon for the Detection of Glutathione

Bing Bian,Xixi Zhu,Qiong Wu,Yue Liu,Shiwei Liu,Qingyun Liu,Shitao Yu

The catalytic activity of nanozymes has attracted much attention in biochemical analyses and the antibiosis and environmental fields. However, easy aggregation and difficulty in recycling greatly result in a decrease of their catalytic activity and further restrict their practical application. Herein, we immobilized Pt and ZnFe2O4 nanoparticles on poplar-wood-derived carbon (ZnFe2O4/C), which exhibited excellent peroxidase-like activity and high affinity toward H2O2 and 3,3′,5,5′-tetramethylbenzidine (TMB). Moreover, it could be easily separated by an external magnetic force from the reaction system. A sensitive and selective colorimetric sensor for glutathione (GSH) was established based on Pt/ZnFe2O4/C nanoperoxidase. The linear range for GSH was from 1 to 30 μM, and the limit of detection for GSH was calculated as 0.38 μM. The colorimetric method was applied to determine GSH in real samples for injection.

研究领域: 生物化学 · 环境科学 · 纳米医学
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DALTON TRANSACTIONS · 2020 ·Vol. 49 ·期 40 ·13999-14008 · IF 4.174

Surface sites assembled-strategy on Pt–Ru nanowires for accelerated methanol oxidation

Mingxuan Li,Yao Wang,Jing Cai,Yunrui Li,Yujie Liu,Yin Dong,Shuna Li,Xiaolin Yuan,Xin Zhang,Xiaoping Dai

Modifying the surface active sites of Pt-based catalysts at the atomic level is of great significance to enhance the electrooxidation of methanol molecules. Herein, efficient active site assembly strategies are proposed, precisely, aimed at building high-performance electrocatalysts. Serving as proof-of-concept examples, both instances of Pt nanowires surface doping isolated Ru atoms (Ru/Pt NWs) and Ru nanoparticles supported on Pt nanowires (Ru@Pt NWs) are specially designed to optimize the catalytic performance of methanol oxidation reaction (MOR). The specific activity and mass activity of optimal Ru/Pt NWs can reach up to 3.93 mA cm−2 and 568.40 mA mg−1Pt, respectively, which is 1.53/1.94 times that of the Ru@Pt NWs and 2.03/2.59 times that of pure Pt NWs. Detailed studies on mechanism reveal that the Pt–Ru alloy can significantly improve the electron transfer kinetics of MOR, and activate more Pt atoms involved in the Langmuir–Hinshelwood (L–H) pathway compared with Ru@Pt NWs, all of which collectively accelerate the methanol oxidation. This surface engineering strategy via assembling active sites can reveal a promising method in the design of advanced Pt-based catalysts for direct methanol fuel cells.

CAS / MDL: 18497-13-7 7601-90-3
研究领域: 材料科学 · 电化学
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FUEL · 2019 · IF 5.128

Preparations and remarkable catalytic cracking performances of Pt@FGS/JP-10 nanofluids

Guozhu Liu,Xueke Jia,Yajie Tian,Siyuan Gong,Li Wang,Xiangwen Zhang

The Pt@FGS/JP-10 nanofluids (0.1 wt% for Pt) were successfully prepared by two consecutive steps: loading Pt nanoparticles on the functionalized graphene sheets (FGS) grafted octadecylamine (ODA) via wet chemical method, following by dispersing it in JP-10 hydrocarbon fuel. The characterization of the prepared Pt@FGS showed that the size of Pt nanoparticles is ca. 2.2 nm, which could be stably dispersed in JP-10 for 2 weeks without significant aggregation or sediment, and the thermal conductivity of 0.2 wt% Pt@FGS/JP-10 nanofluids increases by ca. 35.2% compared with that of pure JP-10. Catalytic cracking performances of Pt@FGS/JP-10 nanofluids were evaluated in a batch reactor heated by fluidized sand at 360–420 °C, and observed that the cracking rate of JP-10 (400 °C, 5 h) improves by 150% in presence of 0.5 wt% Pt@FGS with improved hydrogen selectivity. The possible reason may be attributed to the catalytic dehydrogenation of JP-10 over Pt nanoparticles and the carbon defects on FGS (ca. 71.0% improvement in cracking rate for FGS/JP-10 nanofluids). This work provides a promising method to synchronously improve the thermal conductivity and endothermic cracking rate of JP-10 as a coolant for advanced aircrafts through adding trace Pt@FGS.

研究领域: 材料科学 · 化学工程 · 航空航天工程
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ECS Journal of Solid State Science and Technology · 2022 ·Vol. 11 ·期 4 ·047001 · IF 2.483

Sarcosine Biosensor Based on Pt/g-C3N4 Nanocomposites with High Electrocatalytic Activity

Junyuan Feng,Xiaohui Chen,Xinlin Shi,Weidong Zheng,Xiaofang Zhang,Haipeng Yang

Sarcosine has been shown to be a new biomarker for prostate cancer that is superior to prostate-specific antigen (PSA). By detecting the concentration of sarcosine in the human body, accurate screening and diagnosis of prostate cancer can be achieved in clinical practice. However, the sarcosine level is extremely low in human serum or urine, and accurate detection of sarcosine concentration is difficult. More work is needed to prepare sarcosine biosensors with good anti-interference performance. In this work, we prepared a sarcosine biosensor using a highly electrocatalytically active nanocomposite comprising platinum/carbon nitride (Pt/g-C3N4) as the electrode modification material. The porous lamellar graphite phase carbon nitride (g-C3N4) prevents the agglomeration of Pt nanoparticles and keeps the Pt nanoparticles in a highly dispersed state. The constructed sarcosine biosensor achieves high sensitivity and can selectively detect low concentrations of sarcosine. Its linear detection range is 2–70 μM, and the limit of detection (LOD) is 0.8 μM (S/N = 3). The prepared sarcosine biosensor shows relatively good performance in terms of resistance to interference caused by electroactive substances and provides the potential to be applied in serum for accurate detection of sarcosine.

CAS / MDL: 7722-84-1 108-78-1
研究领域: 生物医学工程 · 肿瘤学 · 分析化学
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Molecular Catalysis · 2024 · IF 3.9

Size control of Pt nanoparticle catalysts for high-selectivity hydrogenation of nitrobenzene to p-aminophenol

Feng Feng,Yaoyao Zhen,Yixin Chen,Jie Luo,Chong Yao,Limei Pan,Ruihao Chen,Jiwei Wu,Chunshan Lu,Xiaoliang Xu,Qingtao Wang,Qunfeng Zhang,Xiaonian Li

Liquid-phase hydrogenation reaction of nitrobenzene to p-aminophenol (PAP) is investigated using a series of Pt-based catalysts, where activated carbon served as support and ethylene glycol (EG) as the reducing agent and solvent. Different platinum sources are employed to obtain Pt/C catalysts with different Pt metal particle sizes, as determined by transmission electron microscopy. The underlying mechanism of nitrobenzene selective hydrogenation on different size of Pt clusters have been systematically investigated. Characterization and catalytic tests show that the catalytic performance of the Pt-based catalyst is deeply influenced by particle size, where the size around 2.5 nm exhibits a suitable hydrogen absorption and activation ability, leading to the best catalytic performance. Under the optimal reaction conditions, the PAP selectivity reached 76.4 % and the conversion of NB reached 100 %. Moreover, the catalyst displayed strong recyclability with the PAP selectivity remaining above 70 % after five cycles of the catalyst, which would enable promising industrial applications.

研究领域: 化学工程 · 催化科学
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IONICS · 2021 ·Vol. 27 ·期 3 ·1221-1231 · IF 2.817

Facile synthesis of coral-like Pt nanoparticles/MXene (Ti3C2Tx) with efficient hydrogen evolution reaction activity

Li Bishan,Ye Rongkai,Wang Qianyu,Liu Xiaoqing,Fang Pingping,Hu Jianqiang

Exploring efficient catalysts for hydrogen evolution reaction (HER) is one of focus points of energy research. In this work, a series of MXene/Pt- x (wherein, x is the adding amount of 6.2 mM H 2 PtCl 6 solution) nanomaterials were fabricated via a facile synthesis method, in which coral-like Pt nanoparticles (NPs) were deposited on Ti 3 C 2 T x MXene. The Pt-loading amounts on the MXene could be simply controlled by varying the adding amounts of H 2 PtCl 6 , which would influence the sizes of Pt NPs on the MXene. The optimum catalytic activity was obtained on the MXene/Pt-3 with a low overpotential of 302 mV versus reversible hydrogen electrode (RHE) at 10 mA cm −2 , which was about 84 mV less than MXene/Pt-2. The efficiently electrocatalytic HER activity of MXene/Pt- x nanomaterials was due to the electron transfer from MXene to Pt NPs. The HER performance of the MXene/Pt- x nanomaterials was influenced by both Pt-loading amounts and Pt particle sizes. This work expands future applications of MXene-based nanomaterials in clean energy conversion reactions.

研究领域: 材料科学 · 能源研究 · 纳米技术
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ACS Sensors · 2024 · IF 8.2

Cu–Pt/CrN Fuel Cell Gas Sensor Achieves ppb-Level H2S Detection at Room Temperature

Huan Wang,Chonghui Zhu,Xiaohui Yan,Zhaorui Zhang,Huashuai Hu,Mengmeng Xu,Yu Liang,Minghui Yang

Fuel cell gas sensors have emerged as promising advanced sensing devices owing to their advantageous features of low power consumption and cost-effectiveness. However, commercially available Pt/C electrodes pose significant challenges in terms of stability and accurate detection of low concentrations of target gases. Here, we introduce an efficient Cu–Pt/CrN-based fuel cell gas sensor, designed specifically for the ultrasensitive detection of hydrogen sulfide (H2S) at room temperature. Compared to the commercial Pt/C sensor, the Cu–Pt/CrN sensor exhibits excellent sensitivity (0.26 μA/ppm), with an increase in the selectivity by a factor of 2.5, and demonstrates good stability over a 2 month period. The enhanced sensing performance can be attributed to the modulation of the electronic arrangement of Pt by Cu, resulting in an augmentation of H2S adsorption. The Cu–Pt/CrN fuel cell gas sensor provides an opportunity for detecting parts per billion-level H2S in various applications.

研究领域: 材料科学 · 传感器技术 · 环境监测
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