DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 38
·13368-13377
·
IF 4.099
Xuefeng Yang,Xiugang Wu,Di Zhou,Junting Yu,Guohua Xie,Duncan W. Bruce,Yafei Wang
Polarised phosphorescence has a bright future in backlighting for conventional liquid crystal displays due to its theoretical 100% internal quantum efficiency and low cost. However, there are scarce reports on polarised phosphorescence from metallomesogens. In this contribution, a platinum-based metallomesogen containing a mesogenic biphenyl (Pt1) was prepared and characterised. To further explore the effect of the substituent on mesophase and emission properties, a related complex Pt2 containing a tetraphenylethene (TPE) moiety was also synthesised. Both complexes melt at elevated temperatures but thereafter do not appear to crystallise on cooling. Complex Pt1 shows an enantiotropic nematic phase from which a broad emission can be seen when spread as a film; in solution, an intense, sky-blue emission is observed. For Pt2, which shows a monotropic SmA phase, the emission in the condensed phase is suppressed and there is only weak emission in solution. Polarisation-dependent photoluminescence with a polarised ratio of 5.4 was obtained for the aligned film of a Pt1:polyimide mixture. Using Pt1 as an emissive layer, non-doped, polarised organic light-emitting diodes presented a broad emission spectrum in the range of 450–900 nm with a polarised ratio of 1.33 and the highest external quantum efficiency of 1.1%. This research has an important significance for achieving broad-based polarised phosphorescence from platinum complex-based metallomesogens.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Naiwei Fu,Ruiyi Wang,Xianmo Gu,Yunwei Wang,Jun Ren,Zhanfeng Zheng
Al 2 O 3 supported Pt nanoparticles photocatalyst enables efficient hydrogen production (115.2 μmol min −1 g cat −1 ) through aqueous phase reforming of methanol (APRM) reaction under light irradiation at low temperatures of 150 °C, which is 6 times higher than that of APRM reaction conducted in the dark. We demonstrate that the particle size of Pt nanoparticles greatly affected the light absorption ability, which is of great importance for light utilization of the photocatalyst. The medium particle size of Pt nanoparticles enables the lower electron density states, which is benefit for the dehydrogenation of methanol and the sequential water–gas shift (WGS) reaction and eventually promoted the photocatalytic performance for hydrogen production.
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Surfaces and Interfaces
·
2022
·
IF 6.137
Kezhong Wu,Zejin Wang,Hui Zhao,Bei Ruan,FeiFei Nie,Rufen Chen,Mingxing Wu
The development of transition metal compounds (TMCs) and conductive polymers composite catalysts substitute for the traditional scarce Pt-based catalysts of counter electrodes (CEs) has been recognized as one of the distinguishing paths to enhance power conversion efficiency (PCE) and decrease manufacturing costs of dye-sensitized solar cells (DSSCs). At present, various thin film preparations have been developed and applied to prepare assortment CEs. Herein, both polyaniline (PANI) and CuWO 4 film were prepared, and further to fabricate layer-by-layer composite CEs of CuWO 4 /PANI, PANI/CuWO 4 , CuWO 4 /PANI/CuWO 4 , PANI/CuWO 4 /PANI, aiming to promote the charge transfer capability and thus improve catalytic activity. And then, PANI, CuWO 4 and four composite layered CEs obtained PCE values of 5.14, 5.64, 5.96, 6.21, 4.96 and 4.24% toward the regeneration of I 3 − /I − redox couples in the assembled DSSCs, respectively. Particularly, the fascinating performance of the bilayer PANI/CuWO 4 CEs inherits the excellent electrical conductivity and the abundant porous structure of PANI skeletons for effective electrolyte diffusion. Meanwhile, the CuWO 4 layer was coupled to the layers of PANI by thermal activation annealing treatment to furnish rich inner active sites for the regeneration of I 3 − /I − couples. Benefit from the synergistic effects of PANI and CuWO 4 , the as-prepared PANI/CuWO 4 CEs manifests the highest PCE of 6.21%, indicating an inspiring strategy by the layered assembly Pt-free CEs with the cost effective and high-performance as an alternative Pt-based catalyst for DSSC.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Meiqi Gao,Junhao Ma,Yanyan Li,Ximao Lin,Limin Wu,Yidong Zou,Yonghui Deng
Hydrogen generation is one of the crucial technologies to realize sustainable energy development, and the design of advanced catalysts with efficient interfacial sites and fast mass transfer is significant for hydrogen evolution. Herein, an in situ coassembly strategy was proposed to engineer a cerium-doped ordered mesoporous titanium oxide (mpCe/TiO2), of which the abundant oxygen vacancies (Ov) and highly exposed active pore walls contribute to good stability of ultrasmall Pt nanoclusters (NCs, ∼ 1.0 nm in diameter) anchored in the uniform mesopores (ca. 20 nm). Consequently, the tailored mpCe/TiO2 with 0.5 mol % Ce-doping-supported Pt NCs (Pt-mpCe/TiO2-0.5) exhibits superior H2 evolution performance toward the water–gas shift reaction with a 0.73 molH2·s–1·molPt–1 H2 evolution rate at 200 °C, which is almost 6-fold higher than the Pt-mpTiO2 (0.13 molH2·s–1·molPt–1 H2). Density functional theory calculations confirm that the structure of Ce-doped TiO2 with Ce coordinated to six O atoms by substituting Ti atoms is thermodynamically favorable without the deformation of Ti–O bonds. The Ov generated by the six O atom-coordinated Ce doping is highly active for H2O dissociation with an energy barrier of 2.18 eV, which is obviously lower than the 2.37 eV for the control TiO2. In comparison with TiO2, the resultant Ce/TiO2 support acts as a superior electron acceptor for Pt NCs and causes electron deficiency at the Pt/support interface with a 0.17 eV downshift of the Pt d-band center, showing extremely obvious electronic metal–support interaction (EMSI). As a result, abundant and hyperactive Ti3+-Ov(-Ce3+)-Ptδ+ interfacial sites are formed to significantly promote the generation of CO2 and H2 evolution. In addition, the stronger EMSI between Pt NCs and mpCe/TiO2-0.5 than that between Pt and mpTiO2 contributes to the superior self-enhanced catalytic performance during the cyclic test, where the CO conversion at 200 °C increases from 72% for the fresh catalyst to 99% for the used one. These findings reveal the subtle relationship between the mesoporous metal oxide-metal composite catalysts with unique chemical microenvironments and their catalytic performance, which is expected to inspire the design of efficient heterogeneous catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Ke Zhang,Xu Zhao,Sihan Chen,Liping Chang,Jiancheng Wang,Weiren Bao,Hui Wang
In chemical cycles to produce hydrogen , the H 2 S splitting cycle and the sulfur-iodine (S I) water splitting cycle both share the Bunsen reaction and HI decomposition. Therefore, they have to overcome the same challenges in the technology development, one of them being the complex and difficult separations of the mixed hydroiodic acid and sulfuric acid solution after the Bunsen reaction. To avoid the separations, this paper studies the electrolysis of the HI/H 2 SO 4 /H 2 O/toluene mixture, focusing on the electrochemical characterization of the Pt electrode by using linear sweep voltammetry (LSV) and cyclic voltammetry (CV). The results show that hydrogen is identified from the gas generated from the cathode in electrolysis. Iodide oxidation is the main reaction in the anode chamber and no significant side reactions are observed. Iodine deposition on the anode surface increases the resistance to iodide diffusion to the anode. However, it can be mitigated by adding toluene in or applying stirring to the anolyte HI/H 2 SO 4 solution. The Pt cathode and sulfuric acid catholyte also work stably.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jie Huang,Yuting Wang,Hangchun Deng,Jianfa Chen,Jianhua Ding,Chunyan Wang
Herein, homogeneously dispersed Pt and MnO 2 nanoparticles were anchored to single-walled carbon nanohorns (SWCNHs) to obtain an efficient electrode material for supercapacitors. XPS and TEM analysis of the Pt/MnO 2 @SWCNH surface morphology confirms that the SWCNHs exhibit a dahlialike cluster structure with Pt/MnO 2 nanoparticles embedded in the interstices of the SWCNH horn structure to form a three-dimensional conductive network. This structure not only improves the overall conductivity of the composite but also provides more electron transfer pathways for the MnO 2 nanoparticles. Accordingly, the as-prepared Pt/MnO 2 @SWCNH composite displays a high specific capacitance (314.5 F/g at 1 A/g), good cycling stability (86.89% capacitance retention after 1000 cycles at 1 A/g), and remarkable rate performance (254.8 F/g at 10 A/g). Among reported composites of metal oxides, precious metals, and carbon materials, the prepared Pt/MnO 2 @SWCNH composite has outstanding electrical properties and is a highly promising candidate as supercapacitor.
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Research
·
2020
·
IF 0
Yiqiong Zhang,Man Qiao,Yucheng Huang,Yuqin Zou,Zhijuan Liu,Li Tao,Yafei Li,Chung-Li Dong,Shuangyin Wang
Direct formic acid fuel cell (DFAFC) has been considered as a promising energy conversion device for stationary and mobile applications. Advanced platinum (Pt) electrocatalysts for formic acid oxidation reaction (FAOR) are critical for DFAFC. However, the oxidation of formic acid on Pt catalysts often occurs via a dual pathway mechanism, which hinders the catalytic activity owing to the CO poisoning. Herein, we directly exfoliate bulk antimony to 2D antimonene (Sb) and in situ load Pt nanoparticles onto antimonene sheets with the assistance of ethylenediamine. According to the Bader charge analysis, the charge transfer from antimonene to Pt occurs, confirming the electronic interaction between Pt and Sb. Interestingly, antimonene, as a cocatalyst, alters the oxidation pathway for FAOR over Pt catalyst and makes FAOR follow the more efficient dehydrogenation pathway. The density functional theory (DFT) calculation demonstrates that antimonene can activate Pt to be a lower oxidative state and facilitate the oxidation of HCOOH into CO2 via a direct pathway, resulting in a weakened intermediate binding strength and better CO tolerance for FAOR. The specific activity of FAOR on Pt/Sb is 4.5 times, and the mass activity is 2.6 times higher than the conventional Pt/C.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2014
·Vol. 18
·期 9
·2487-2496
·
IF 2.234
Wang Zhihua,Li Jinshu,Xu Lijuan,Feng Yanjun,Lu Xiaoquan
A sensitive and selective imprinted electrochemical sensor for the determination of aflatoxin B 1 (AFB 1 ) was constructed on a glassy carbon electrode by stepwise modification of functional multiwalled carbon nanotubes (MCNTs), Au/Pt bimetallic nanoparticles (Au/PtNPs), and a thin imprinted film. The fabrication of a homogeneous porous poly o -phenylenediamine (POPD)-grafted Au/Pt bimetallic multiwalled carbon nanotubes nanocomposite film was conducted by controllable electrodepositing technology. The sensitivity of the sensor was improved greatly because of the nanocomposite functional layer; the proposed sensor exhibited excellent selectivity toward AFB 1 owing to the porous molecular imprinted polymer (MIP) film. The surface morphologies of the modified electrodes were characterized using a scanning electron microscope. The performance of the imprinted sensor was investigated by cyclic voltammetry, differential pulse voltammetry, and electrochemical impedance spectroscopy in detail. A linear relationship between the sensor response signal and the logarithm of AFB 1 concentrations ranging from 1 × 10 −10 to 1 × 10 −5 mol L −1 was obtained with a detection limit of 0.03 nmol L −1 . It was applied to detect AFB 1 in hogwash oil successfully.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Zixuan Xie,Hu Cheng,Zhuo Chen,Xiaotong Yang,Zhiyou Zhou,Qiang Yuan
The development of multimetallic Pt-based nanostructures as high-performance cathodic electrocatalysts to be used in water-splitting devices for hydrogen generation is the focus of increasing attention. In this study, a family of hierarchical architectures constructed from dendritic quaternary PtFeRuRh, ternary PtFeRh or PtFeRu and binary PtFe nanoalloys are achieved via a general liquid-phase strategy for hydrogen evolution in alkaline electrolyte . Among them, the PtFeRuRh nanoalloys exhibit the lowest overpotential (20.0 mV at 10 mA cm −2 ) and Tafel slope (21.1 mV dec −1 ). At a potential of −0.07 V, the mass activity of the PtFeRuRh nanoalloy is 7.04 A mg Pt −1 , it is 6.97 times that of commercial Pt/C. The dendritic PtFeRuRh nanoalloys exhibit a negligible decrease in activity after 20 h of continuous testing at 10 mA cm −2 /100 mA cm −2 and 3000 cyclic voltammetry cycles. In a practical application, the cell voltage of a PtFeRhRu (−) || IrO 2 (+) couple is 1.568 V at 10 mA cm −2 with almost 100% faradaic efficiency. The turnover frequency of the PtFeRhRu electrocatalyst at 70 mV was 78.5 s −1 , which is 11.71 times as large as that of commercial Pt/C (6.7 s −1 ).
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Zhengshan Gao,Xiang Liu,Chengli Zhang,Zhiyong Tang,Jun Chen,Chao Yu
A novel label-free electrochemical sensing strategy for detecting monocyte chemoattractant protein-1 (MCP-1) was developed by using single-walled carbon nanohorns (SWCNHs) functionalized with Pt nanoparticles (PtNPs-SWCNHs). After modification with the PtNPs-SWCNHs, the electrode could serve as an effective platform for antibody immobilization and electron transfer owing to the large surface area and excellent conductivity of PtNPs-SWCNHs. Moreover, the PtNPs-SWCNHs composite could provide an obvious electrochemical signal through amperometric i–t curve method, due to its high catalytic activity for the reduction of hydrogen peroxide (H 2 O 2 ). Under optimal conditions, the amperometric i-t curve signals had a strong linear relation with the logarithm of the MCP-1 concentration ranging from 0.06 pg mL -1 to 450 pg mL -1 , and the detection limit was 0.02 pg mL -1 . Furthermore, the proposed immunosensor could detect MCP-1 in serum samples with desirable results. Overall, this immunosensor may provide a new alternative strategy for rapid detection of MCP-1.
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ChemNanoMat
·
2022
·Vol. 8
·期 10
·e202200268
·
IF 3.82
Mengmeng Liu,Jingjing Li,Pengfei Wang,Shuai Chen,Zhengping Dong,Fengwei Zhang
Graphical The encapsulation of Pt/TiO 2 -450H catalyst with SMSI into zeolite silicalite-1 (S-1) is reported. The resulting Pt/TiO 2 @S-1 catalyst dispalyed superior catalytic performance especially for halogenated nitroaromatics and without degradation in selectivity after 7 cycles. It is attributed to the high surface area, SMSI effect in confined space and the pore structure of S-1 with selective adsorption of substrates. The encapsulation of metal nanoparticles (NPs)-based active sites and homogeneous catalysts in nanoporous materials has been of highly research focus for tuning their catalytic activity, selectivity and stability. Although the catalysts with strong metal-support interaction (SMSI) hold the reversible encapsulation feature in a certain atmosphere, there is still a lack of systematic research on them in a real confined environment. Herein, we present a highly selective and stable Pt/TiO 2 @S-1 catalyst, which is prepared by in-situ growth of classical silicalite-1 on the external surface of Pt/TiO 2 -450H pre-catalyst with SMSI effect. Encouragingly, the encapsulated 20Pt/TiO 2 @S-1 catalyst demonstrates unprecedented catalytic performance for various nitroaromatics and without any degradation in selectivity after 7 cycles (>99%) for the hydrogenation of 1-chloro-4-nitrobenzene. Such situation is attributed to the high surface area, SMSI effect in confined space as well as the pore structure of silicalite-1 with selective adsorption of substrates.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Min Song,Ming Chen,Chang Zhang,Jingjing Zhang,Wei Liu,Xiao Huang,Jingwen Li,Guang Feng,Deli Wang
The atomic ensemble effect will affect the catalysis on catalyst surfaces and determine the selectivity of multielectron reactions, which is an effective potential strategy to modulate the oxygen reduction reaction (ORR) selectivity for hydrogen peroxide (H2O2) production. Here, we reported the investigation of the ensemble effect on Pt/Pd chalcogenides for the two-electron ORR. A series of Pt/Pd chalcogenides were synthesized via introducing chalcogens into Pt/Pd, resulting in catalysts with isolated Pt/Pd active site. X-ray adsorption spectroscopy reveals the change of the electronic structure. Their ORR selectivity transformed from a four-electron process to a two-electron one, which was attributed to the isolated active sites changing the adsorption mode and the tunable electronic property weakening the adsorption energy. Density functional theory calculations revealed that Pt/Pd chalcogenides possessed a lower binding energy of OOH* and inhibited the breakage of the O–O bond, and PtSe2/C with an optimal adsorption energy of OOH* showed 91% selectivity toward H2O2 production. This work provides a design principle for synthesizing highly selective Pt group catalysts for H2O2 production.
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