CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zhiyuan Liu,Linmeng Wang,Changan Wang,Rushuo Li,Peiyun Zhou,Hongyi Gao,Ge Wang
Strong metal-support interaction (SMSI) plays an important role in heterogeneous catalysis, but the influence of the chemical microenvironment of metal on it is often neglected. In this study, a mesoporous Ce-MOFs with pyridine N sites and open metal sites (OMS) were constructed, and highly dispersed Pt nanoclusters (NCs) and Pt-N x interface were subsequently introduced and constructed via SMSI effect for hydrogenation of dicyclopentadiene (DCPD). The spectroscopic results and density functional theory (DFT) computations demonstrate that pyridine N and OMS can regulate the SMSI effect between Ce-PyDC and Pt through Pt-N x interface and electronic interaction between Pt and OMS, which increase electron cloud density of Pt nanoclusters, promote DCPD adsorption, H 2 activation. The optimal Pt NCs@Ce-PyDC-3 can efficiently convert DCPD to tetrahydrodicyclopentadiene (THDCPD) at 50 °C, giving a 100 % DCPD conversion and 99 % THDCPD selectivity. This work provides an in-depth understanding of the correlation between the metal nanoparticle microenvironment and SISM effect.
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Chemosensors
·
2022
·Vol. 10
·期 7
·260
·
IF 4.229
Zhaoxia Shi,Ling Xia,Gongke Li,Yufei Hu
High purity methyl tert-butyl ether (MTBE) can be used to adjust gasoline octane values. However, an isomer, methyl sec-butyl ether (MSBE), is the main by-product of its industrial production, and this affects the purity of MTBE. Pt/Au NPs@Co3O4composites with a hollow dodecahedron three-dimensional structure were synthesized using ZIF-67 as a template, with Pt and Au nanoparticles (NPs) evenly distributed on the shell of the hollow structure. A CTL sensor was established for the determination of MSBE based on the specificity of Pt/Au NPs@Co3O4. The experimental results showed that Pt/Au NPs@Co3O4had a strong specific cataluminescence (CTL) response to MSBE, with no interference from MTBE. The linear range was 0.10–90 mg/L, the limit of detection was 0.031 mg/L (S/N= 3), the RSD was 2.5% (n= 9), and a complete sample test could be completed in five minutes. The sensor was used to detect MSBE in MTBE of different purity grades, with recoveries ranging from 92.0% to 109.2%, and the analytical results were consistent with those determined by gas chromatography. These results indicate that the established method was accurate and reliable, and could be used for rapid analysis of MTBE gasoline additive.Keywords:Pt/Au NPs@Co3O4;cataluminescence sensor;methyl sec-butyl ether;methyl tert-butyl ether;rapid analysis;gasoline additive
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高影响因子
Materials Today Chemistry
·
2022
·
IF 7.613
W. Zhan,L. Ma,M. Gan
Herein, we report an efficient bottom-up approach to construct the carbon encapsulated CoP nanoarray-like architectures onto the nitrogen-doped Ti 3 C 2 MXene Pt-based catalyst (Pt–CoP@CNT NA/N–Ti 3 C 2 ) by employing metal-organic frameworks (MOFs) as the sacrificial template. Benefiting from the catalytic effect for metals into MOFs and synergistic effect of Ti 3 C 2 substrate, homogenous nanotubes nanoarray-like structure is obtained on Ti 3 C 2 nanosheet . The unique heteroatom-doped 3D connected structure endows the catalyst with distinct structural merits, such as the carbon and nitrogen-enriched structures, large specific surface areas and excellent conductivity, leading to the high dispersion of ultrafine metallic Pt and efficient electronic/mass transfer, contributing to more exposed active sites of Pt surface. The fabricated CoP and doped nitrogen especially for those lattice nitrogen derived from the pristine MOFs can present exceptional co-catalytic effect, resulting in obtaining strong anti-CO poisoning capacity for catalyst. Therefore, the ultrahigh catalytic activity of per Pt active site for methanol oxidation reaction can be preserved. Besides, owing to the strong stability of carrier, the catalyst delivers a reliable long-term stability during the test. This work gives new ideal for the design of novel cost-effective 3D Ti 3 C 2 -based nanomaterial catalyst with excellent catalytic activity for methanol oxidation.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Fuyuan Qi,Weiping Yang,Haochen Yu,Lan-Lan Lou,Shuangxi Liu,Kai Yu
The electronic interaction between metal and support plays a significant role in varying catalytic activity of oxide-supported metal catalysts for the aerobic oxidation of biomass-based alcohols and aldehydes. Employing Y 3+ -doped ceria supported Pt catalysts, Pt/Ce 1-x Y x O 2-δ , different interfacial atomic structures, including Pt/Ce-Vo(-Ce) 2 , Pt/Y-Vo(-Ce) 2 , Pt/Ce-Vo(-Y) 2 , and Pt/Y-Vo(-Y) 2 (Vo represents an oxygen vacancy), were created in this work to modulate the interfacial electron transfer capacity. The results of experimental and theoretical investigations showed that the Pt/Y-Vo(-Ce) 2 interfacial structure owned the highest electron transfer capacity from Pt to the support, resulting in more Pt δ+ /Y-Vo(-Ce) 2 sites. Accordingly, the catalyst Pt/Ce 0.75 Y 0.25 O 2-δ owning the largest amount of Pt δ+ /Y-Vo(-Ce) 2 sites exhibited notably promoted catalytic activity for the oxidation of 5-hydroxymethylfurfural (HMF) toward 2,5-furandicarboxylic acid (FDCA), affording a complete conversion of HMF and 96.6% yield of FDCA in 6 h. This work provided a facile and versatile strategy to modulate the electron transfer capacity of oxide supported metal catalysts by manipulating the interfacial atomic structure for promoting their activities in various catalytic oxidation reactions.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Yangyang Wang,Xiaoxia Liu,Annie Yang,Ping Lv,Lixin Zhang,Yongnian Li,Yanzhao Yang
Selective recovery of gold and platinum from secondary resources is of great significance under the crisis of resource shortage. Hence, the optimal extractant 1-(2-(dimethylamino) ethyl)-4-methyl-piperazin bis(trifluoromethylsulfonyl)imide ([C 6 -Et-TMEDA-PIP][Tf 2 N] 2 ) was synthesized and screened out from five piperazine-based ionic liquids (ILs) to construct an IL-water system for Au(III) and Pt(IV) extraction. ILs have high hydrophobicity and low viscosity at room temperature, which can be used as both extractant and hydrophobic phase. The effects of IL dosage, metal concentration and acidity on the extraction efficiency were investigated. Under the optimal conditions, the extraction efficiency of 98.5% (Au(III)) and 97.5% (Pt(IV)) can be achieved. The anion exchange mechanism was verified through the combination of Ultraviolet visible spectroscopy (UV–vis), Nuclear magnetic spectra (NMR) and quantum chemical calculations. Besides that, the two-factor optimization of the extractant dosage and HCl concentration was carried out by Response surface methodology (RSM), and the effective separation of Au(III) and Pt(IV) was successfully achieved. Au(III)/ Pt(IV) was extracted into the IL phase as [Et-TMEDA-PIP + ][AuCl 4 - ] and can easily be stripped by reduction to Au(0)/Pt(Ⅱ) with H 2 C 2 O 4 /CS(NH 2 ) 2 -HCl, and each extraction ability maintained after 5 turns of extraction cycle experiments. Since the excellent behaviors showed in the multi-metal selective extraction and cycle experiments, the [C 6 -Et-TMEDA-PIP][Tf 2 N] 2 was regarded as the most potential system for Au(III) and Pt(IV) recovery from HCI medium.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Shuang Li,Jiawei Zhang,Cherie S. Tan,Chong Chen,Chang Hu,Yongchang Bai,Dong Ming
As important biomarkers for prostate cancer, total prostate specific antigen (tPSA) and free prostate specific antigen (fPSA) levels in serum play essential roles in early diagnosis. In this study, hybrid molybdenum disulfide (MoS 2 )/Pt@Au-nanoprism/polydopamine (PDA)-modified screen-printed electrodes were utilized to detect both fPSA and tPSA in serum simultaneously. MoS 2 generated by the hydrothermal method assembled on the electrode to provide binding sites for further modification. Au nanoprisms were obtained by reducing chloroauric acid with sodium thiosulfate to achieve uniformity. Pt nanoparticles covered on Au nanoprisms by the displacement method, and the generated Pt@Au-nanoprism structure was then deposited onto the electrode to enhance the electrochemical signals. An electropolymerization-synthesized PDA film further modified the electrode to increase antibody binding sites. The results demonstrated that the proposed electrochemical immunosensor for fPSA and tPSA analysis in serum using differential pulse voltammetry (DPV) had a wide linear range from 0.0001 ng/mL to 100 ng/mL, with limits of detection (3 SD/slope) at 0.1 pg/mL and 1.1 fg/mL, respectively. For clinical patient samples, the proposed biosensor demonstrated good accuracy according to the clinical electrochemiluminescence immunoassay and improved the diagnostic specificity of tPSA concentrations in the “gray zone", suggesting promising prospects for clinical applications of our multiplex biosensors.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 36
·期 5
·e6646
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IF 4.072
Yanyun Wang,Yuming Zhou,Jiehua Bao,Jiajia Wang,Yiwei Zhang,Xiaoli Sheng,Yuzhong Huang
Pt nanocatalysts have received enthusiastic attention in the field of clean energy technologies due to their high catalytic activity and selectivity. The growth size and dispersion of Pt particles play significant effects on the reaction activity, especially in high temperature catalytic reactions where catalysts are prone to deactivation due to agglomeration and sintering of Pt particles. Herein, the Pt nanoparticles were effectively stabilized on AIPO-18 molecular sieve by a biomolecule-mediated green synthesis method. Based on the biocompatibility and electrostatic synergy of carboxymethyl chitosan (CMC), a high degree of Pt nanoclusters dispersion in AIPO-18 zeolites was achieved. The hydroconversion of levulinic acid (LA)was carried out at 160°C and 2 MPa hydrogen pressure, and the LA conversion of Pt/AIPO-18 (5CMC) reached 95.2% and the selectivity of γ-valerolactone (GVL) was 97.9% after 2 h. Pt/AIPO-18 (5CMC) exhibited satisfactory results that superior to the initial reactivity of Pt/AIPO-18 (0CMC) after five runs.
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MICROCHEMICAL JOURNAL
·
2021
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IF 4.821
Ruru Wang,Xuerui Liu,Yiwei Zhao,Jianhua Qin,Hui Xu,Lina Dong,Shanmin Gao,Linlin Zhong
A novel carbon composite was integrated with Au@Pt core–shell nanoparticles (Au@Pt NPs) to construct a sensing interface for enzyme-free electrochemical detection of glucose. As surfactant, graphene oxide (GO) was used to disperse multi-walled carbon nanotubes (MWCNTs). After the glassy carbon electrode (GCE) was modified with the mixture of GO and MWCNTs, the Au@Pt NPs were decorated on it. The prepared novel three-dimensional sensor interface was applied to detect glucose without enzyme at a remarkable negative potential (at about −0.013 V vs. Ag/AgCl), demonstrating a low detection limit (4.2 × 10 −8 M) and two wide linear range from 5 × 10 −8 to 1 × 10 −4 M and 1 × 10 −4 M to 2.5 × 10 −3 M. In addition, the non-enzymatic glucose sensing platform can be realized for practical application.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Libin Shi,Yiming Zhou,Xiao Tan,Suitao Qi,Kevin J. Smith,Chunhai Yi,Bolun Yang
The morphologies and the electron property of catalysts play the very important roles in the hydrogenation and dehydrogenation of liquid organic hydrogen carriers (LOHCs) such as dibenzyltoluene (DBT). The different morphologies and pore structures of γ-Al 2 O 3 and Mo x C doped γ-Al 2 O 3 were synthesized as the supports for Pt catalysts. After analyzing of various characterizations and catalytic testing, it was found that the large surface area and the mesoporous structure of catalysts are beneficial to both DBT hydrogenation and perhydro-dibenzyltoluene (H18-DBT) dehydrogenation. The doping of Mo x C promoted the formation of the smaller Pt nanoparticles and increased Pt dispersion. The forming Pt–Mo structure is beneficial to hydrogen spillover which suppress the formation of by-product. The high Pt dispersion of 0.1 wt% Mo x C doped Pt/Al 2 O 3 catalyst plays the positive roles in increasing H18-DBT dehydrogenation activity.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiabin Shen,Shanshan Xu,Cheng Zhao,Xiaopeng Qiao,Haiquan Liu,Yong Zhao,Jing Wei,Yongheng Zhu
In this work, we present a new metal oxide semiconductor gas sensor for detecting trimethylamine (TMA) by bimetal Au@Pt-modified α-Fe2O3 hollow nanocubes (NCs) as sensing materials. The structure and morphological characteristics of Au@Pt/α-Fe2O3 were evaluated through multiple analyses, and their gas-sensitive performance was investigated. Compared with the pristine α-Fe2O3 NC sensor, the sensor based on Au@Pt/α-Fe2O3 NCs exhibited faster response time (5 s) and higher response (Ra/Rg = 32) toward 100 ppm TMA gas at a lower temperature (150 °C). Furthermore, we also assessed the Au@Pt/α-Fe2O3 NC sensor for detecting the freshness of Larimichthys crocea which have been observed by headspace solid-phase microextraction and gas chromatography–mass spectrometry. The high performance of the Au@Pt/α-Fe2O3 NCs is attributed to the special hollow morphology with a high specific surface area (212.9 m2/g) and the synergistic effect of the Au@Pt bimetal. The Au@Pt/α-Fe2O3 sensor shows promising application prospects in estimating seafood freshness on the spot.
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PubMed
高影响因子
BIOELECTROCHEMISTRY
·
2023
·
IF 5
Mengjiao Zhu,Yu Liu,Meiyue Wang,Tao Liu,Zhenyu Chu,Wanqin Jin
Owing to the high mortality and strong infection ability of COVID-19, the early rapid diagnosis is essential to reduce the risk of severe symptoms and the loss of lung function. In clinic, the commonly used detection methods, including the computed tomography (CT) and reverse transcription-polymerase chain reaction (RT-PCR), are often time-consuming with bulky instruments, which normally require more than one hour to report the results. To shorten the analytical period for testing the COVID-19 virus (SARS-CoV-2), we proposed an ultrafast and ultrasensitive DNA sensors to achieve an accurate determination of the DNA sequence by the RNA reverse transcription (rtDNA) of the SARS-CoV-2. A nanocubic architecture of the MnFe@Pt crystals was constructed to integrate both electrocatalysis and conductivity to greatly improve the biosensing performance. After the immobilization of a specific capture and report DNA on above nanocomposite, the rtDNA can be rapidly caught to the DNA sensor to form a double-helix structure, thus generating the current signal change. Within only 10 min, the as-prepared DNA sensors exhibited ultralow detection limit (1 × 10 −20 M) and wide linear detection range, together with an outstanding selectivity among various interfering substances.
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高影响因子
FOOD CHEMISTRY
·
2023
·
IF 8.8
Jingjuan Wang,Juan Wu,Mimi Sun,Jing Bai,Xiangjie Bo
This study presents the first integrated electrochemical platform (IEP) with point-of-use and portable features for on-site determination of ponceau 4R (RP), amaranth (AM), and tartrazine (TZ) in food by integrating a mass-producible Pt nanoparticles/laser-engraved graphene (Pt NPs/LEG)-based sensing chip and a reusable electrochemical miniaturized workstation. The sensing chip utilizes Pt NPs/LEG with unique architectures as electrode material and exhibits desirable analytical performance towards RP, AM, or TZ with satisfied linear range (0.25–50 μM for RP, AM, and TZ), high sensitivity (7.29 μA μM −1 cm −2 , 7.18 μA μM −1 cm −2 , and 2.02 μA μM −1 cm −2 for RP, AM, and TZ, respectively) and low limit of detection (50 nM, 58 nM, and 204 nM for RP, AM, and TZ, respectively). The sensing chip shows excellent selectivity, high stability, outstanding reproducibility, and acceptable mechanical stability. IEP can be implemented to test RP, AM, or TZ in real samples with satisfactory accuracy and recoveries.
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