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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

In-situ Bi-modified Pt towards glycerol and formic acid electro-oxidation: Effects of catalyst structure and surface microenvironment on activity and selectivity

Xiaomei Ning,Liang Zhan,Xiaosong Zhou,Jin Luo,Yanli Wang

The performances of glycerol electro-oxidation reaction (GOR) and formic acid electro-oxidation reaction (FAOR) catalyzed by Pt catalyst were dramatically improved by adding Bi 3+ into the reaction solution. The dynamic structure and microenvironment of in-situ Bi-modified Pt and their impact on the catalytic performances were revealed. A strong correlation was established between the Bi coverage of Pt-based catalysts and their resistance to CO poisoning and performance in GOR and FAOR. When Bi 3+ increased to a certain amount, a Bi-shell containing hydroxides was formed on Pt surfaces except the formation of Pt-Bi ensemble. On Pt catalyst covered with 43.9 % Bi, the peak mass-specific activities of GOR and FAOR in forward scans were 4.2 and 34.7 times that of Pt/NCNTs, respectively. The peak electrochemical active surface area (ECSA)-specific activity of FAOR in forward scan for Pt with 52.6 % Bi coverage was 80.6 times that of Pt/NCNTs. The dehydrogenation process in FAOR and the 4-electron pathway in GOR were improved for Bi-modified Pt. The experimental results and DFT calculations indicated that the positively charged Bi and structure of Pt-Bi ensemble improved the adsorption and interaction of negatively charged intermediates, and the enhanced hydroxides facilitated the oxidation and removal of toxic intermediates, such as CO.

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Foods · 2023 ·Vol. 12 ·期 17 ·3319 · IF 5.2

A Multi-Enzyme Cascade Response for the Colorimetric Recognition of Organophosphorus Pesticides Utilizing Core-Shell Pd@Pt Nanoparticles with High Peroxidase-like Activity

Zainabu Majid,Qi Zhang,Zhansen Yang,Huilian Che,Nan Cheng

In modern agricultural practices, organophosphorus pesticides or insecticides (OPs) are regularly used to restrain pests. Their limits are closely monitored since their residual hinders the capability of acetylcholinesterase (AChE) and brings out a threatening accumulation of the neurotransmitter acetylcholine (ACh), which affects human well-being. Therefore, spotting OPs in food and the environment is compulsory to prevent human health. Several techniques are available to identify OPs but encounter shortcomings like time-consuming, operating costs, and slow results achievement, which calls for further solutions. Herein, we present a rapid colorimetric sensor for quantifying OPs in foods using TMB as a substrate, a multi-enzyme cascade system, and the synergistic property of core-shell Palladinum@Platinum (Pd@Pt) nanoparticles. The multi-enzyme cascade response framework is a straightforward and effective strategy for OPs recognition and can resolve the previously mentioned concerns. Numerous OPs, including Carbofuran, Malathion, Parathion, Phoxim, Rojor, and Phosmet, were successfully quantified at different concentrations. The cascade method established using Pd@Pt had a simple and easy operation, a lower detection limit range of (1–2.5 ng/mL), and a short detection time of about 50 min. With an R2value of over 0.93, OPs showed a linear range of 10–200 ng/mL, portraying its achievement in quantifying pesticide residue. Lastly, the approach was utilized in food samples and recovered more than 80% of the residual OPs.Keywords:Pd@Pt nanoparticles;organophosphorus pesticides;acetylcholinesterase;colorimetric detection;multi-enzyme cascade

CAS / MDL: 67-68-5
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Confined tuning of the charge distribution of Pt electrocatalyst for reinforcing anti-poisoning ability: Toward efficient separation of hydrogen from gases containing ammonia

Changqing Jin,Fanglin Wu,Haibo Tang,Hongfei Pan,Zhida Chen,Rui Wang,Zihan Meng,Junsheng Li,Haolin Tang

The development of catalysts for hydrogen oxidation reaction (HOR) with enhanced resistance to ammonia poisoning is an important factor in the practical application of hydrogen electrochemical purification devices (HEPDs). This paper reports on the creation of a highly active and anti-ammonia HOR catalyst developed by tuning the charge distribution of the support material through nitrogen-doping of carbon. The nitrogen-doped carbon-supported platinum catalyst (Pt-N 2 /KB, 2.03 wt% Pt) achieves a high mass activity and exchange current density of 2788 mA mg pt -1 and 1020 mA mg pt -1 , respectively, which are 5.4 and 4.7 times higher than that of the comm. 20% Pt/C. The Pt-N 2 /KB catalyst also displays a lower percentage of current decay and enhanced electrochemical stability, indicating superior anti-ammonia toxicity in the tests with HEPD. Density functional theory (DFT) calculations reveal that the hydrogen adsorption free energy (ΔG H* ) on the surface of Pt-N 2 /KB is close to zero and has a lower ammonia adsorption energy, thus accounting for its superior HOR activity and anti- ammonia poisoning ability. Consequently, this work facilitates the implementation of HOR catalysts for anti-ammonia poisoning in the HEPDs, thus accelerating the advancement of ammonia cracking for hydrogen production .

CAS / MDL: 64-17-5 461-58-5
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FOOD AND AGRICULTURAL IMMUNOLOGY · 2021 · IF 3.101

A sensitive biomimetic enzyme-linked immunoassay method based on Au@Pt@Au composite nanozyme label and molecularly imprinted biomimetic antibody for histamine detection

Xiaofeng Wang,Yongfeng Chen,Runze Yu,Ruiqiang Wang,Zhixiang Xu

In this paper, a sensitive biomimetic enzyme-linked immunoassay (BELISA) method based on an Au@Pt@Au composite nanozyme label was developed for histamine (HA) detection. A molecular imprinted polymer prepared directly on the 96-well plate served as a biomimetic antibody. A BELISA method was developed for HA standard solutions at concentrations ranging from 0.01 to 100.00 mg/L. Under optimal conditions, the novel BELISA method had a low limit of detection (0.069 mg/L) and high sensitivity (7.20 mg/L). The HA spiked in yellow rice wine and liqueur samples were detected by this BELISA method with the recoveries ranging from 84.28% to 108.82%. There was no significant difference of the results between the BELISA method and HPLC for the detection of HA in the red and white grape wine samples.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Facile electrolytic synthesis of Pt and carbon quantum dots coloaded multiwall carbon nanotube as highly efficient electrocatalyst for hydrogen evolution and ethanol oxidation

He Xiao,Shoufeng Xue,Jingjuan Zhang,Man Zhao,Jianchun Ma,Shuai Chen,Zhanfeng Zheng,Jianfeng Jia,Haishun Wu

Designing high-performance Pt-based catalysts with low catalysts cost is still a great challenge. Here, we demonstrate a facile electrolysis-solvothermal technique for making Pt and carbon   quantum   dots coloaded multiwall carbon nanotube (Pt-CQDs/MWCNT) catalyst with the assistant of electric   field. Despite of the ultralow Pt amount (0.81 wt%) for the optimized Pt-CQDs/MWCNT catalyst, it exhibits ultrahigh electroactivity and durability toward hydrogen evolution reaction (HER) and ethanol oxidation reaction (EOR). The mass activities of the catalyst for HER and EOR can be achieved to 4889.7 mA/mg (-40 mV) and 4917 mA mg −1 Pt (forward peak), which are 8.1 times and 5.6 times more active than those of commercial Pt/C respectively. The characterization results reveal that Pt nanpparticles (Pt NPs) with intrinsic structure play the key role in excellent catalytic performance for HER and EOR. CQDs not only support abundant anchoring points for fixation and dispersion of Pt NPs, but also construct 3D conductive network with MWCNT supporter for improving the catalytic performance.

CAS / MDL: 68-12-2 108-32-7
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APPLIED CATALYSIS A-GENERAL · 2020 · IF 5.006

A novel viewpoint on the surface adsorbed oxygen and the atom doping in the catalytic oxidation of toluene over low-Pt bimetal catalysts

Yankun Du,Jianwu Zou,Yang Guo,Xiang Xu,Hongyu Chen,Changqing Su,Zheng Zeng,Liqing Li

The low-Pt bimetal compounds (PtNi 3 -C and PtFe 3 -C) were synthesized via the chemical reduction method and the toluene catalytic oxidation experiments were conducted to test their catalytic performance. The sample of PtFe 3 -C (T 100  = 255 ℃) possessed a better low-temperature catalytic activity than PtNi 3 -C (T 100  = 288 ℃) due to a higher content of Pt (0), while both two catalysts had a desirable catalytic stability (⁓100 % within 72 h). The reaction kinetic parameters were acquired from the Mars-van Krevelen (MVK) model, and the MVK mechanism combined with the in-situ DRIFT was used to investigate the reaction pathway. Moreover, the theoretical calculations based on DFT was applied to study the accessibility of toluene to the surface of metal atoms doping. Herein, this study not only can provide a promising catalyst with the superior low-temperature catalytic activity and stability, but also can give a comprehensive understanding on the toluene catalytic oxidation mechanism over bimetal catalysts.

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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2020 ·Vol. 95 ·期 6 ·1756-1772 · IF 2.75

Construction of Z-scheme Pt-TiO2/(Er3+:Y3Al5O12@Ta2O5)/HAP and its application in sonocatalytic degradation of prometryn and disinfection of Escherichia coli

Guanshu Li,Yuejiao Cao,Ludong Yi,Jun Wang,Youtao Song

BACKGROUND The recovery and reuse of sonocatalysts are the pivotal issues in the sonocatalytic degradation of organic pollutants. The use of some natural minerals as the carrier is not only beneficial to recycling of sonocatalysts, but also reduces the treatment costs of organic pollutants. Two kinds of hydroxyapatite (HAP), Ox Bone (OB)-HAP and synthesized (Syn)-HAP combine with the Pt-TiO 2 /(Er 3+ :Y 3 Al 5 O 12 @Ta 2 O 5 ) (P-TET) composite, obtaining two Z-scheme sonocatalysts, P-TET/OB-HAP and P-TET/Syn-HAP, respectively. The sonocatalytic activities of the prepared samples are investigated via degradation of prometryn and disinfection of Escherichia coli . RESULTS A series of characterizations showed that the Z-scheme P-TET/(OB or Syn)-HAP sonocatalysts were prepared successfully. To evaluate their sonocatalytic activities, some influencing factors such as ultrasonic irradiation time, inorganic oxidants, used times and trapping agents on the sonocatalytic degradation prometryn were determined. The best degradation ratio (80.31% based on N computing and 85.07% based on S atom computing) of prometryn could be obtained for 10 mmol L −1 K 2 S 2 O 8 , 1.0 g L −1 P-TET/OB-HAP sonocatalyst and 150 min ultrasonic irradiation. The excellent sonocatalytic disinfection ratio (88.65%) of E. coli could also be obtained under 40 min ultrasound irradiation. Moreover, a possible mechanism on sonocatalytic degradation of prometryn was illustrated. CONCLUSION The treated bovine bone HAP was directly used as a carrier to combine with P-TET to construct a novel Z-scheme P-TET/OB-HAP sonocatalyst. The high degradation ratio of prometryn and disinfection ratio of E. coli showed that P-TET/OB-HAP could be a promising sonocatalyst for the degradation of organic pollutants and the disinfection of bacteria. © 2020 Society of Chemical Industry

CAS / MDL: 7287-19-6
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Theranostics · 2020 · IF 8.579

Point-of-care assay for drunken driving with Pd@Pt core-shell nanoparticles-decorated ploy(vinyl alcohol) aerogel assisted by portable pressure meter

Yu Zhang,Quanyi Liu,Chong-Bo Ma,Qingqing Wang,Meiting Yang,Yan Du

Alcohol abuse causes health problems and security accidents. A reliable and sensitive detection system for alcohol has been an instinctive demand in law enforcement and forensic. More efforts are demanded in developing new sensing strategy preferably with portable and non-invasive traits for the pushforward of point-of-care (POC) device popularization. Methods : We developed a POC diagnosis system for alcohol assay with the aid of alcohol oxidase (AOX) pre-joining in the system as well as Pd@Pt core-shell nanoparticles (abbreviated to Pd@Pt) that were decorated on ploy(vinyl alcohol) aerogel with amphiphilicity. Biological samples like saliva and whole blood can be absorbed by the aerogel in a quick process, in which the analyte would go through a transformation from alcohol, H 2 O 2 , to a final production of O 2 , causing an analyte dose-dependent signal change in the commercial portable pressure meter. The cascade reactions are readily catalyzed by AOX and Pd@Pt, of which the latter one possesses excellent peroxidase-like activity. Results : Our design has smartness embodied in the aerogel circumvents the interference from methanol which is more ready to be catalyzed by AOX. Under the optimal conditions, the limit of detection for alcohol was 0.50 mM in saliva, and is able to distinguish the driving under the influence (DUI) (1.74 mM in saliva) and driving while impaired (DWI) (6.95 mM in saliva) in the national standard of China. Conclusion : Our proof-of-concept study provides the possibility for the establishment of POC device for alcohol and other target detection, not only owing to the sensing qualification but also thanks to the architecture of such sensor that has great flexibility by replacing the AOX with glucose oxidase (GOX), thenceforth realizing the accurate detection of glucose in 0.5% whole blood sample. With the advantages of easy accessibility and anti-interference ability, our sensor exhibits great potential for quantitative diagnostics in biological system.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Facile synthesis of novel spherical covalent organic frameworks integrated with Pt nanoparticles and multiwalled carbon nanotubes as electrochemical probe for tanshinol drug detection

Cong Zhang,Min Cui,Jujie Ren,Yifei Xing,Na Li,Haiyan Zhao,Peng Liu,Xueping Ji,Meng Li

In this work, a novel spherical covalent organic frameworks (COFs) was developed via a simple and facile room-temperature solution route. Via in situ growth of Pt nanoparticles (PtNPs) on the surface of COFs, PtNPs@COFs composites with improved electroactivity were successfully prepared. After incorporation of MWCNTs into the composites, the PtNPs@COFs-MWCNTs nanocomposites that possess excellent electrical conductivity and unprecedented catalytic performance were formed and utilized as novel electrode materials for fabrication of an electrochemical tanshinol sensor. Under the optimum conditions, this electrochemical sensor presented excellent electrochemical properties to tanshinol with a wide linear range from 0.002 to 1.1 mM, a high sensitivity up to 10.089 μA mM −1 , and a low detection limit (LOD) of 0.018 μM (S/N = 3). Moreover, due to the high selectivity, excellent stability and good repeatability, the constructed sensor was successfully applied to measure the amount of tanshinol in real medicinal samples with satisfactory results. Our findings pave the way to utilize COFs as the structural component for design of sensing platforms and extend the applications of COFs in catalysis, analysis and drug testing.

CAS / MDL: 92-87-5 34374-88-4
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Molecular Catalysis · 2021 · IF 5.062

Enhanced hydrogen evolution reaction activity of FeM (M = Pt, Pd, Ru, Rh) nanoparticles with N-doped carbon coatings over a wide-pH environment

Guoliang Gao,Huangze Yu,Xue Lu Wang,Ye-Feng Yao

The alloy catalyst formed by transition metal and a small amount of noble metal has become the most promising substitute for M-based ( M  = Pt, Pd, Ru, Rh) catalyst. However, due to the direct exposure of the metal core to the electrolyte, it is vulnerable to corrosion and oxidation, which in turn reduces the catalytic stability and is becoming a major obstacle to sustainable hydrogen production. The present work addresses this issue by developing a one-step immersion-adsorption-pyrolysis strategy for synthesizing FeM alloy nanoparticles with N-doped carbon coatings (FeM@CN) for use as electrocatalysts in the HER. The deliberately designed metal-organic framework material was used as the precursor of catalyst synthesis to achieve the carbon coatings and simultaneously the heteroatom in-situ doping for the alloy nanoparticles. The optimal FePt@CN demonstrates excellent catalytic stability and HER activity in an acidic electrolyte medium. The reactions obtain a small overpotential of 28 mV to achieve current densities of 10 mA cm −2 , which are comparable to a high-performance commercial Pt/C electrocatalyst with a much higher Pt loading. The FeRu@CN also demonstrates an outstanding performance with an overpotential of only 18 mV to achieve a current density of 10 mA cm −2 in an alkaline medium.

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JOURNAL OF CATALYSIS · 2019 · IF 7.723

Highly efficient Pt-Co alloy hollow spheres with ultra-thin shells synthesized via Co-B-O complex as intermediates for hydrogen evolution reaction

Min Wei,Lei Huang,Shangli Huang,Zhenyu Chen,Dandan Lyu,Xiaoran Zhang,Shuangbao Wang,Zhi Qun Tian,Pei Kang Shen

Improving utilization of precious metals is one of the crucial challenges for electrochemical energy catalysis. Tuning precious metal structure to expose active sites is an effective strategy to reduce mass loading in the practical application. Herein, Pt-Co hollow nanospheres were synthesized via a sequential reduction strategy using amorphous Co-B-O complex as the key spheres-forming intermediates. The modulation mechanism of Pt-Co hollow nanospheres formation was established by investigating critical factors of addition sequence of reducing agent, the type of reducing agents and the ratio of Pt and Co precursors. The optimized Pt-Co hollow nanospheres with the Pt/Co molar ratio of 1:1 by this method is characterized by the average diameter of around 30 nm and the shell thickness of 2.3 nm. They displays superior performance for enhanced hydrogen evolution reaction (HER) in the aspect of activity and stability in 0.5 M H 2 SO 4 , in which the mass activity of the Pt-Co hollow spheres exhibits 2.82 times higher than that of commercial Pt/C and its stability also has a significant enhancement. The outstanding activity of the Pt-Co hollow nanospheres for HER is mainly attributed to its highly accessible electron/mass transport path, expose active sites on the ultra-thin shells and strain effect induced by the hollow sphere structure. This hollow nanospheres with ultra-thin shell provides a promising way to develop highly efficient precious metal based electrocatalysts.

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JOURNAL OF CATALYSIS · 2018 · IF 6.759

Significance of surface oxygen-containing groups and heteroatom P species in switching the selectivity of Pt/C catalyst in hydrogenation of 3-nitrostyrene

Qifan Wu,Bin Zhang,Chao Zhang,Xiangchun Meng,Xinluona Su,Shan Jiang,Ruhui Shi,Yan Li,Weiwei Lin,Masahiko Arai,Haiyang Cheng,Fengyu Zhao

The selectivity of 3-nitrostyrene (NS) hydrogenation over 0.5 wt-% Pt catalysts supported on carbon materials can be switched simply by changing reduction temperature. When the reduction temperature was 150 °C, 1-ethyl-3-nitrobenzene (ENB) was mainly produced in a selectivity of 93% at a conversion of 95% (at 100 °C). When the reduction was conducted at a higher temperature of 450 °C, in contrast, the main product was switched to 3-aminostyrene (AS) in a selectivity of 96% at a conversion of 91%. That is, the Pt/C catalysts reduced at low and high temperatures could preferentially catalyze the hydrogenation of vinyl and nitro groups of NS, respectively. This switching of the product selectivity may be ascribed to actions of surface oxygen-containing functional groups and surface hetero P species. The quantity and nature of these surface species were examined in detail by a few different methods. For the low-temperature reduced catalyst, surface acidic groups present close to Pt nanoparticles (∼2 nm) would interact with the nitro group of a NS molecule and make its vinyl group more likely to interact with the surface active metal species of Pt nanoparticles; this facilitates the hydrogenation of the latter and produces ENB selectively. For the high-temperature reduced catalyst, however, P species would interact with Pt and form Pt-PO x complex, on which a NS molecule is likely to be adsorbed with its nitro group, facilitating the selective production of AS via its hydrogenation. It is demonstrated that surface functional groups and surface hetero atoms (like P), in addition to main active metal species (like Pt), should have direct actions in the catalysis for such a catalyst that exposes a larger quantity of surface functional groups and/or hetero atoms compared to the number of supported metal nanoparticles .

CAS / MDL: 83-86-3
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