JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaotong Yang,Kaiyu Dong,Zhe Zheng,Yuehuan Zhang,Qiang Yuan
Efficient C C bond cleavage and the complete oxidation of alcohols are key to improving the efficiency of renewable energy utilization. Herein, we successfully prepare porous Fe-doped hexagonal close-packed ( hcp )-PtBi/face-centered cubic ( fcc )-Pt heterostructured nanoplates with abundant grain/phase interfaces ( h -PtBi/ f -Pt@Fe 1.7 PNPs) via a simple solvothermal method. The open porous structure, abundant grain/phase interface and stacking fault defects, and the synergistic effect between intermetallic hcp -PtBi and fcc -Pt make h -PtBi/ f -Pt@Fe 1.7 PNPs an effective electrocatalyst for the glycerol oxidation reaction (GOR) in direct glycerol fuel cells (DGFCs). Notably, the h -PtBi/ f -Pt@Fe 1.7 PNPs exhibit an excellent mass activity of 7.6 A mg Pt −1 for GOR, 4.75-fold higher than that of commercial Pt black in an alkaline medium. Moreover, the h -PtBi/ f -Pt@Fe 1.7 PNPs achieve higher power density (125.8 mW cm −2 ) than commercial Pt/C (81.8 mW cm −2 ) in a single DGFC. The h -PtBi/ f -Pt@Fe 1.7 PNPs can also effectively catalyze the electrochemical oxidation of 1-propanol (17.1 A mg Pt −1 ), 1,2-propanediol (7.2 A mg Pt −1 ), and 1,3-propanediol (5.2 A mg Pt −1 ). The in-situ Fourier-transform infrared spectra further reveal that the C C bond of glycerol, 1-propanol, 1,2-propanediol, and 1,3-propanediol was dissociated for the complete oxidation by the h -PtBi/ f -Pt@Fe 1.7 PNPs. This study provides a new class of porous Pt-based heterostructure nanoplates and insight into the intrinsic activity of different C3 alcohols.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yi-Hu Ke,Xiao-Mei Yu,Xue Wang,Hai Liu,Hong Yuan
Accurately controlling the directional activation of the primary and secondary hydroxyls and preventing the deep oxidation of oxygen-containing functional groups and the degree of C–C cleavage is still a great challenge for the selective oxidation of glycerol to glyceric acid. Hence, a series of bimetallic Au-Pt/M x O y C z catalysts (M = Cu, Co, Ce, Mn, Ni, Zn, Zr) were prepared using MOFs-derived transition metal carbon-based compounds as the support. These catalysts were utilized for glycerol catalytic oxidation to glyceric acid under basic conditions. The experimental date indicated that the type of transition metal makes a big difference on the conversion of glycerol and the selectivity of glyceric acid under the mild condition of 60 ℃. Among them, the Mn-modified carbon-based compound supported Au-Pt/Mn x O y C z catalyst has the best catalytic activity. After reaction for 2 h, the conversion of glycerol could reach 100 %, and the selectivity of glyceric acid could reach 57.3 %. The reason for the best activity of the Au-Pt/Mn x O y C z catalyst is that the particle size of active molecules is small, and the strong metal-support interaction produces more active sites. Specifically, Au-Pt/Mn x O y C z catalyst forms an Au-Pt alloy, and the synergy between alloyed Au-Pt and Mn &+ enhances the acidity of the catalyst, causing it to produce the most acidic sites and promoting the dispersion of metal nanoparticles. The strong basic site of the catalyst can promote Au-Pt electron transfer, which in turn changes the reducing properties of Au-Pt and enriches the oxygen vacancies of the catalyst. Therefore, the synergistic interaction between the acidic sites and strong basic sites promotes the activation of Au-Pt, which in turn promotes the reduction of Mn-based oxides and the activation and migration of oxygen. This work will offer some new recommendations for the development of MOFs-derived transition metal-based catalysts for the catalytic oxidation of bio-polyols under mild conditions.
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ADVANCED MATERIALS
·
2024
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IF 27.4
Yu Zhang,Qin Zhao,Bukhvalov Danil,Weiping Xiao,Xiaofei Yang
The Pt-based alloys can moderate the binding energies of oxygenated species on the catalytic surface, endowing the superior catalytic performance towards oxygen reduction reaction (ORR). Nevertheless, it is still challenging to explore general methods to synthesize structurally ordered intermetallics with uniform distributions. Herein, the strong metal-support interaction is employed to facilitate the interdiffusion of Pt/M atoms by establishing a tunnel of oxygen vacancy on ultrathin Ti 3 C 2 T x (MXene) sheets, synthesizing the ordered PtFe, PtCo, PtZn, PdFe, PdZn intermetallics loaded onto Ti 3 C 2 T x . Furthermore, the in-situ generation of Ti–O from Ti 3 C 2 T x could be bonded with Pt and forming Pt–O–Ti, resulting in charge redistribution through Pt–O–Ti structure. Theoretical calculations demonstrate that the valuable charge redistribution can be observed at the interface and extended even to at the distance of two nanometers from the interface, which can modulate the Pt–Pt distance, optimize Pt–O binding energy and enhance intrinsic activity towards ORR. The strong coupling interaction between PtFe and Ti 3 C 2 T x containing the titanium oxide layer endows the high stability of the composites. This work not only presents a general synthesis strategy for intermetallics but also provides a new insight that metal-support interaction is essential for the structural evolution of intermetallics on materials with oxygen vacancies.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 32
·期 3
·e4208
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IF 3.581
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.
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ANALYTICA CHIMICA ACTA
·
2018
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IF 5.123
Yamin Fu,Di Huang,Congming Li,Lina Zou,Baoxian Ye
This paper described a novel, facile and nonenzymatic electrochemical biosensor to detect hydrogen peroxide (H 2 O 2 ). The sensor was fabricated based on Pd-Pt nanocages and SnO 2 /graphene nanosheets modified electrode (PdPt [email protected] /GCE). The electrochemical behavior of PdPt [email protected] /GCE exhibited excellent catalytic activity toward H 2 O 2 with fast response, high selectivity , superior sensitivity, low detection limit of 0.3 μM and large linear range from 1 μM to 300 μM. Under these obvious advantages, the constructed biosensor provided to be reliable for determination of H 2 O 2 secreted from human cervical cancer cells (Hela cells). Hence, the proposed biosensor is a promising candidate for detection of H 2 O 2 in situ released from living cells in clinical diagnostics.
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Green Energy & Environment
·
2025
·
IF 14.6
Jinshan Chen,Jiangfeng Lu,Ran Lang,Chi Wang,Shuangyou Bao,Yuan Li,Kai Li,Maohong Fan
In this study, a novel Pt-loaded CuPc/g-C 3 N 4 (PtCuCN) composite was synthesized for the selective photocatalytic reduction of CO 2 to CH 4 under visible light. The PtCuCN catalyst achieved a CH 4 yield of 39.8 μmol g⁻ 1 h⁻ 1 , significantly outperforming bulk g-C₃N₄ and CuPc alone by factors of 2.5 and 3.1, respectively, with a high selectivity of 90%. In comparison with other commonly studied photocatalysts, such as g-C 3 N 4 -based catalysts, the PtCuCN composite exhibited superior CH 4 yield and product selectivity, demonstrating its potential as a more efficient photocatalyst for CO₂ reduction. X-ray photoelectron spectroscopy (XPS), density functional theory (DFT) calculations, and in-situ infrared (IR) analysis revealed that the Pt⁰ species effectively lower the activation energy for CH 4 formation, while CuPc extends the light absorption range and enhances charge separation. The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO 2 -to-CH 4 photocatalysts. This work demonstrates the potential of PtCuCN as a highly efficient and stable catalyst for CO 2 reduction to CH 4 under visible light.
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BIOSENSORS & BIOELECTRONICS
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2010
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IF 5.429
Shujun Ji,Qingqing Guo,Qiaoli Yue,Lei Wang,Huaisheng Wang,Jinsheng Zhao,Ruixin Dong,Jifeng Liu,Jianbo Jia
Fabrication of sub-monolayer array of Pt nanoparticles (PtNPs) assembled at nucleobases terminated layers and their application into H 2 O 2 and glucose sensing were reported. To prepare such a PtNPs assembly, 3-mercaptopropionic acid (MPA), Zr 4+ , nucleotide-5′-monophosphate (NTMP including guanosine, adenosine, cytidine, uridine-5′-monophosphate, and abbreviations were GMP, AMP, CMP, UMP, respectively) were adsorbed onto Au substrate sequentially to form nucleobases terminated surface and Zr 4+ acted as binder to link carboxylic and phosphoric groups (NTMP/Zr 4+ /MPA/Au). Complexation of cisplatin, cis-Pt(NH 3 ) 2 Cl 2 , with terminated nucleobases and following electrochemical reduction of surface-bound cisplatin gave PtNPs attached surface. Different PtNPs coverage or particle density was obtained depending on the NTMP used and decreased in the order: PtNPs/GMP/Zr 4+ /MPA/Au > PtNPs/AMP/Zr 4+ /MPA/Au > PtNPs/CMP/Zr 4+ /MPA/Au > PtNPs/UMP/Zr 4+ /MPA/Au. The surface loading of Pt was between 160 and 16 ng/cm 2 . The as prepared PtNPs can be used as electrocatalysts for H 2 O 2 sensing (detection limit of H 2 O 2 < 100 nM) and the sensitivity increased with decreasing PtNPs density. After adsorption of glucose oxidase, the modified electrode can be used as enzymatic electrode for glucose sensing and a detection limit of 38.5 μM was achieved. This study provided an example of fabricating PtNP arrays utilising surface complexation of cisplatin with nucleobases. The advantage of this method is that the NP density can be controlled through changing nucleobases or Pt complexes used to obtain suitable kinetics of the complexation reactions. Additionally, the PtNPs sub-monolayer as prepared has high sensitivity for H 2 O 2 sensing even at a very low loading of Pt.
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ANALYTICAL CHEMISTRY
·
2009
·
IF 5.712
Jingming Gong,Ting Zhou,Dandan Song,Lizhi Zhang,Xianluo Hu
A new, highly sensitive and selective sensor for the electrochemical assay of Hg(II) by anodic stripping voltammetry has been developed, whereby a glassy carbon electrode is modified with a novel inorganic−organic hybrid nanocomposite, namely, bimetallic Au−Pt nanoparticles/organic nanofibers (labeled as Au−PtNPs/NFs). The sensor possesses a three-dimensional (3D) porous network nanoarchitecture, in which the bimetallic Au−Pt NPs serving as metal NP-based microelectrode ensembles are homogenously distributed in the matrix of interlaced organic NFs. The surface structure and composition of the sensor were characterized by scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). Its electrochemical performance was systematically investigated. Our results show that such a newly designed, Au−PtNPs/NF nanohybrid modified electrode provides remarkably improved sensitivity and selectivity for the stripping assay of Hg(II). The detection limit is found to be as low as 0.008 ppb (S/N = 3) that is much below the guideline value from the World Health Organization (WHO). Interferences from other heavy metal ions such as Cu(II), Cr(III), Co(II), Fe(II), Zn(II), and Mn(II) ions associated with mercury analysis are effectively inhibited. Toward the goal for practical applications, the sensor was further evaluated by monitoring Hg(II) in tap and river water specimens.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Xiaohong Tan,Wenzhan Li,Wei He,Tingting Yu,Bingbing Wan,Yong Huang,Jintao Liang,Guiyin Li
Glypican-3 (GPC3), which is a surface heparan sulfate proteoglycan, has been widely known the ideal biomarker for diagnosis and treatment of hepatocellular carcinoma (HCC). Accurate and sensitive detection of serum GPC3 level is an important and challenging task. In this paper, a sandwich electrochemical aptasensor was designed to specifically detect serum GPC3 level through aptamer-target-aptamer recognition. A GPC3 aptamer (GPC3 Apt ) immobilized on the surface of gold nanoparticles@reduced graphene oxide modified screen-printed electrode (Au NPs@rGO/SPCE) was used as the capture probe. Hemin-reduced graphene oxide-carboxymethyl chitosan@platinum nanoparticles (H-rGO-CMC@Pt NPs), with good mimicking peroxidases activity, were labeled with amination GPC3 aptamer, which was employed as the signal probe. Once the target GPC3 was anchored on the surface of GPC3 Apt /Au NPs@rGO/SPCE, the H-rGO-CMC@Pt NPs-GPC3 Apt was further specifically bound to the GPC3, forming the aptamer-target-aptamer sandwich structure, which can catalyze the oxidation of hydroquinone (HQ) to benzoquinone (BQ) and lead the oxidation current of HQ recorded by DPV to changing. The linear relationship between the current signal of oxidation of HQ and GPC3 concentration range of 0.0001–3.0 µg/mL and 3.0–60.0 µg/mL, with a low detection limit (LOD) of 0.0685 ng/mL. Additionally, the electrochemical aptasensor was successfully applied for the detection of GPC3 in human serum samples with the recovery of 99.95–104.06 % and relative standard deviation (RSD) of 1.31–5.22 %. Thus, the sandwich aptasensor could provide a new strategy for detection of serum GPC3 level and improve the early diagnosis rate of HCC.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinyuan Zhou,Qiyan Sun,Xinlin Wang,Ruixue Zhang,Bin Li,Zexing Wu,Dehong Chen,Lei Wang,Guang-Rui Xu
Synthesis of cost-effective electrocatalysts for oxygen reduction reaction (ORR) has received wide attention due to their sluggish kinetics, which limits the development and application of fuel cell technique. In this work, we report a versatile synthetic approach to prepare a series of small-sized Ag@MNi (M = Pd, Pt, Rh, Ru) nanocrystals with core–shell structures by a simple solvothermal method. According to characterization analysis, surface segregation of Pd was proved in the outermost layer with the Pd-rich shell layer, which can regulate the adsorption energy of *OH. Electrochemical results show that the onset potential and half-wave potential of Ag@PdNi nanocrystals (Ag@PdNi NCs) are 1.005 and 0.913 V vs. RHE (reversible hydrogen electrode), respectively, with a Tafel slope of 55.31 mV dec -1 and strong ORR catalytic durability, which is similar to Ag@MNi (M = Pt, Rh, Ru) NCs and slightly higher than that of PdAg alloy nanoparticles (PdAg alloy NPs), PdNi alloy nanoparticles (PdNi alloy NPs), commercial Pd black and even commercial Pt/C, in alkaline medium. Density Functional (DFT) calculations show that the presence of Ag core effectively promotes the segregation of Pd atoms to the outer shell surface, where Ni provides better segregated substitution sites for Pd, which significantly improves the ORR activity and durability due to the electronic synergistic effect between Ag core nuclei and Pd shell can reduce the adsorption strength of OH ads .
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Analytical Methods
·
2024
·
IF 2.7
Taohong Zhou,Jin Lin,Fengmei Jin,Yanxing Yao,Zhihao Li,Lihua Wang
Cr(VI) is one of the most typical heavy metal contaminants and rapid detection of Cr(VI) is highly important in food control and public health. Herein, a core–shell Au@Pt nanozyme-based colorimetric assay was developed for the rapid and sensitive detection of Cr(VI). The monodispersed Au@Pt core–shell nanoparticles exhibited high peroxidase-mimicking activity and can catalyze colorless TMB into blue-colored oxidized oxTMB. After the addition of Cr(VI), the oxTMB molecules can be reduced into colorless TMB. The ultrathin Pt shell can prevent the Pt component from aggregation, thus improving the catalytic activity of Au@Pt nanozyme. These Au@Pt nanozyme-based Cr(VI) assays exhibited high sensitivity and selectivity and displayed satisfactory recoveries in practical samples. Our work highlights opportunities for the development of core–shell nanozymes with extensive applications in food safety, biomedicine, and environmental monitoring.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shuxiu Yang,Qingzhu Shu,Bona Fu,Shuhong Liu,Yong Zhang,Hong Zhao
One important approach to address the cost issue of fuel cells is to maximize the utilization of Pt by reducing its loading and enhancing the performance for the oxygen reduction reaction (ORR) as well as durability of catalysts. In this work, a one-step synthesis of highly dispersed low-Pt (1 1 1) electrocatalysts (p-Pt/KBs) supported by Ketjenblack is conducted using interaction between solution and nonthermal plasma (SNP). The results show that the plasma-treated platinum precursor dispersion efficiently avoids particle agglomeration and increases more defects of the support surface, which are conducive to the trapping and anchoring of platinum nanoparticles (Pt NPs). The catalyst (p-Pt/KB-NaOH) with a platinum load of 10.8 wt% is obtained by adding sodium hydroxide to the platinum precursor dispersion solution, showing better ORR performance (E 1/2 = 0.88 V) and stability compared to the commercial platinum on carbon (Pt/C) catalyst (20 wt%, E 1/2 = 0.86 V). This improvement is attributed to the fact that neutralizing chloroplatinic acid slows down the reduction rate of the platinum precursor, effectively controlling the rapid nucleation and slow crystal growth of platinum. As the cathode catalyst for PEMFCs, p-Pt/KB-NaOH exhibits remarkable mass-transfer performance in the high-current density domain (HCD), with maximum power density (P max ) of 1131 mW cm −2 at 2500 mA cm −2 , which is 9.1 % higher than commercial Pt/C. Moreover, the single-cell operates stably for at least 100 h at 1000 mA cm −2 with a negligible decay (1.9 %) of the working voltage, ensuring long-term durability.
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