INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Mingxia Song,Bofeng Zhang,Ziwei Zhai,Sibao Liu,Li Wang,Guozhu Liu
Atomically dispersed metal catalysts can maximize the utilization of metals and provide unique chemical properties for catalytic reactions. However, the stabilities of high-loading metal clusters on solid supports are still under dispute, because small clusters are prone to agglomerate into larger particles at high temperature. Here, we prepared thermally stable highly dispersed Pt species immobilized by bridging Zn2+ sites and silanol groups (Si-OH) on self-pillared silicalite-1 zeolite nanosheets (SP-S-1). The rotationally overgrown zeolite sheet-like structure provided a high specific surface area and abundant Si-OH, which favored atomically dispersed active sites with ZnOx-Si nanoclusters. The as-prepared PtZn/SP-S-1 exhibited a high specific activity of 1.23 molC3H6·gcatal–1·h–1 at 580 °C with propylene selectivity up to 99%. Moreover, no obvious deactivation was observed after 90 h on stream under a weight hourly space velocity of 15 h–1. The self-pillared nanosheet-supported metal catalysts provide prospective guidance for high-temperature catalysis.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Shuqi Hu,Yuying Liu,Shuangbao Wang,Xinyi Zhang,Pei Kang Shen
Design and synthesis of platinum catalysts within atomic level are of great significance for the practical application of fuel cells. We found that the ultrathin Co(OH) 2 nanoparticles can be converted into Co 3 O 4 –Co core-shell nanostructures through a thermal annealing process in reducing atmosphere, which are uniformly distributed on the surface of 3D graphene (3DG). The Co 3 O 4 –Co core-shell nanoparticles have been successfully transformed into Co 3 O 4 –Pt core-shell nanoparticles via a controlled replacement reaction. The Co 3 O 4 –Pt @3DG contains only a few atomic layers of Pt shell, and presents a high Pt utilization nanostructure. Besides, the 3D graphene serves as a catalysts carrier with open structure, and offers a three-dimensional molecular accessibility and conducive to mass transfer. Significantly, the optimized mass activity and specific activity of 1.018 A/mg Pt and 2.17 mA/cm 2 have been achieved on Co 3 O 4 –Pt @3DG at 0.9 V vs RHE , which are 7.6- and 8.1- times higher than those of Pt/C (0.134 A/mg Pt and 0.266 mA/cm 2 ), respectively. The high activity is mainly attributed to the ultrathin core-shell structure with an ultrahigh Pt utilization, and the interaction between the near-surface Co 3 O 4 and the surface Pt shell with a tensile strain to surface Pt shell, and the electrons transfer from Co to Pt.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2019
·Vol. 412
·期 2
·521-530
·
IF 3.286
Li Yuzhen,Yang Lingling,Xu Jing,Zhou Hairihan,Gao Zhida,Song Yanyan
Nanomaterials that exhibit enzyme-like activity (nanozymes) have attracted significant attention due to their potential for applications in analytical tests and in the biological field. In this study, an enzyme-like nanomaterial is developed by coupling Pt nanoparticles with WO 2.72 (Pt/WO 2.72 ). The resultant nanocomposite nanomaterial exhibits peroxidase activity and catalase activity. Moreover, owing to the presence of W 6+ and W 5+ in WO 2.72 , Pt/WO 2.72 nanoplates demonstrate promise as scavengers of hydroxyl radicals. The Pt/WO 2.72 composite nanoplates exhibit excellent peroxidase-like activity for the sensitive colorimetric detection of H 2 O 2 and blood glucose. These Pt/WO 2.72 nanoplates are thought to be a promising tool for broad potential applications in biomedicine, biotechnology, and environmental chemistry.
Pt nanoparticles anchored WO 2.72 nanoplates (Pt/WO 2.72 ) as a multienzyme-like mimetics exhibits peroxidase activity and catalase activity. Furthermore, this composite can be acted scavengers of hydroxyl radicals.
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DYES AND PIGMENTS
·
2017
·
IF 3.473
Yuan Zhao,Xuan Yang,Linyan Cui,Yali Sun,Qijun Song
Mercury ions (Hg 2+ ) and silver ions (Ag + ) are assigned to the highest toxicity class of heavy metal pollution. Here, a novel sensor is firstly developed for the simultaneous detection of coexisting Ag + and Hg 2+ in aqueous solution, depending on the catalytic properties of poly(vinyl pyrrolidone) (PVP)-capped platinum nanoparticle (Pt NPs) and the strong chelation of EDTA to Hg 2+ . PVP-capped Pt NPs exhibit uniform morphology and possess great intrinsic peroxidase-like activity in comparison to citrate-capped Pt NPs, PVP-capped Ru NPs and Ir NPs, attributing to the enhanced catalytic efficiency determined by loosely packed PVP and the excellent catalytic decomposition activities of H 2 O 2 . Hg 2+ and Ag + could induce remarkable inhibition of the peroxidase-like activity of Pt NPs by changing the electronic state of the active sites through metallophilic interactions. The selective and simultaneous detection of Hg 2+ and Ag + was realized via the addition of ethylenediaminetetraacetate (EDTA), which could successfully mask Hg 2+ but had negligible effect on Ag + . The proposed approach inspires new designs of novel catalytic nanoprobes for the multi-analyte assay of heavy metal ions .
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Science China-Chemistry
·
2022
·Vol. 65
·期 10
·2038-2044
·
IF 10.138
Wang Yanan,Pei Chunlei,Zhao Zhi-Jian,Gong Jinlong
Rational design and performance promotion are eternal topics and ultimate goals in catalyst preparation. In contrast, trial—and—error is still the common method people take. Therefore, it is important to develop methods to intrinsically enhance the performance of catalysts. The most effective solutions are the one from a kinetic perspective based on clear knowledge of the reaction mechanism. This paper describes rate-determining step cognition and modulation to promote CO oxidation on highly dispersed Pt on CeO 2 . The different degrees of metal—support interactions due to variation of hydroxyl density of support could alter the structure of active species and the ability of oxygen activation apparently, further shift the rate-determining step from oxygen activation to oxygen reverse spillover kinetically. The transformation of rate-determining step could enhance the intrinsic activity significantly, and decrease the T 50 approximately 140 °C. The findings of this research exemplify the universal and effective method of performance elevation by rate-determining step modulation, which is promising for application in different systems.
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DYES AND PIGMENTS
·
2015
·
IF 3.966
Tianchu Zhao,Rui Liu,Hong Shi,Mingliang Shu,Jinyang Hu,Huan Li,Hongjun Zhu
A series of 4-phenyl-2,2′; 6′,2″-terpyridyl Pt(II) complexes bearing different σ -alkynyl ancillary ligands ( 1a – 1f ) were synthesized and characterized. All complexes exhibit strong 1 π , π * absorption bands in the UV region; and broad, structureless metal-to-ligand charge transfer ( 1 MLCT)/ligand-to-ligand charge transfer ( 1 LLCT) absorption bands in the visible region. When excited at the charge-transfer absorption band, the complexes exhibit yellow to red luminescence ( λ max = 553–608 nm) in CH 3 CN at room temperature, which is attributed to the 3 MLCT/ 3 LLCT state, except 1c . The emitting state of 1c exhibits a significant intraligand 3 π , π * character, which is originated from the naphthalimide acetylide ligand. Complexes 1a – 1c exhibit moderate triplet transient absorptions from visible to NIR region, where reverse saturable absorption (RSA) occurs. The photophysical, electrochemical and nonlinear absorption properties of these Pt(II) complexes can be tuned drastically by the different acetylide ligand, which would be useful for rational design of broadband nonlinear absorption materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Yuhui Li,Enze Zhu,Juan Yu,Jie Yu,Jirong Yang,Weiping Liu,Xiaoyin Cui,Xikun Yang,Yingjie Zhang,Mingli Xu
A novel carbon fiber paper loaded with reduced graphene oxide (rGO) was used as the substrate, on which Pt–Ni nanoparticles were electro-deposited as to prepare an integrated electrode by two electrochemical methods (cyclic voltammetry and square wave pulse). The electrochemical tests indicated two integrated electrodes had excellent performance towards methanol oxidation . Especially, Pt-Ni-CV(A)-rGO/CFP electrode showed the highest electrocatalytic activity , and mass activity reached 5.33 A·mg −1 Pt , which was about 5.6 times that of the commercial Pt/C catalyst (JM). Further, after annealing under a reducing atmosphere, two electrodes exhibited completely different changes in the aspects of morphology and electrocatalytic performance. It can be attributed to the changes of element distribution and morphology of nanoparticles after annealing. The as-prepared Pt–Ni-rGO/CFPs composite electrode is promising for integrated electrode of proton exchange membrane fuel cells. This work opens an avenue for the preparation of high-performance integrated electrode.
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ChemCatChem
·
2021
·Vol. 13
·期 18
·3953-3959
·
IF 5.686
Zhiming Zhou,Hongyan Jia,Yong Guo,Yangang Wang,Xiaohui Liu,Qineng Xia,Xi Li,Yanqin Wang
Graphical Sulfates : The introduction of sulfates into TiO 2 supported Pt-WO x catalyst greatly improves the dispersion of Pt and WOx species, increases the acid amount and inhibits the leaching of Pt and WO x species, resulting in dramatically promoted catalytic activity and stability for glycerol hydrogenolysis to 1,3-PDO and n-PO with 93 % total yield. Pt-WO x based catalysts were widely investigated and showed high industrial application potential for glycerol hydrogenolysis. Further improving the catalytic activity and stability of the Pt-WO x based catalysts is important. Herein, we modified the TiO 2 supported Pt-WO x catalyst with sulfate doping and employed for the glycerol hydrogenolysis. The introduction of sulfates dramatically promoted the catalytic activity and stability of the Pt/W/Ti catalyst in glycerol hydrogenolysis. Sulfates-doped Pt/W−S/Ti achieved 100 % conversion of glycerol, with 36 % selectivity to 1,3-PDO and 57 % selectivity to n-PO at 120 °C and 4 MPa, while the conversion over Pt/W/Ti only reached 57 %. Moreover, Pt/W−S/Ti offered 22.5 times more glycerol conversion (90 %) than Pt/W/Ti (4 %) for the second run. The much higher activity of the Pt/W−S/Ti was ascribed to the better dispersion of Pt and WO x species and more Brønsted acid amount. The enhanced stability of Pt/W−S/Ti was attributed to its strong anti-leaching ability after sulfate doping.
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Nature Communications
·
2025
·
IF 15.7
Yi Li,Chen Chaohao,Wen Yingjie,Zhang Sixie,Chen Haocheng,Zhu Jinchao,Weng Jiabin,Zhang Wuyong,Xu Wenwen,Guan Wanbing,Chen Xu,Qiu Tianyu,Tian Xinlong,Lu Zhiyi
The electrochemical synthesis of solid compounds is a critical emerging area in electrocatalysis; however, a major challenge is still remaining on severe catalysts scaling driven by strong solid-solid interactions, giving rise to rapid electrode deactivation. In this study, for the example of simultaneous synthesis of Mg(OH) 2 and H 2 from natural seawater electrolysis, we demonstrate that Pt catalyst with surface-coordinated halogens (F, Cl, Br, I) can alleviate this scaling effect (i.e., solidophobicity) by like-charge repulsion and thus regulating the local environment. Specifically, Pt-I coordination results in supersolidophobicity, achieving a successful extraction of Mg(OH) 2 ( > 99% purity) while stably producing H 2 (under 100 mA cm -2 for over 5000 hours). A combination of experimental and theoretical studies reveals that, due to the like charge repulsion between I - and in situ generated OH - , the Pt-I catalyst regulates the surface pH gradient which increases the distance from the electrode surface to the Mg(OH) 2 nucleus (>4 μm) and facilitates homogeneous nucleation. Additionally, the scalability of the Pt-I catalyst, along with the techno-economic analysis and life cycle assessment of the natural seawater electrolysis technology are systematically demonstrated.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Bo Li,Peng Sun,Ruoyu Zhang,Zhenyu Wang,Zonghua Wang
The electrocatalytic hydrogen evolution reaction (HER) is widely recognized as a promising pathway for sustainable energy conversion and storage. Recently, plasmonic enhancement has attracted increasing attention as an effective strategy to improve HER performance by harvesting incident light. However, most metal nanoparticles (NPs) with excellent HER catalytic activity, such as Pt, exhibit a negligible localized surface plasmon resonance (LSPR) effect, thereby limiting their overall efficiency. In this study, we constructed a Pt NPs–Ti3C2 MXene hybrid electrocatalyst via an in situ reduction approach, in which Ti3C2 MXene simultaneously acted as the reductant, structural support, and plasmonic mediator. Under 808 nm laser irradiation, Ti3C2 MXene generated a strong LSPR effect, and the resulting hot electrons were efficiently injected into the Pt NPs/Ti3C2 MXene interface, where they actively contributed to the HER process. Consequently, the hybrid catalyst achieved an overpotential as low as 51 mV at 10 mA cm–2 and a favorable Tafel slope of 61.29 mV dec–1 while maintaining excellent stability. Finite element simulations further confirmed that the LSPR-induced local field enhancement concentrated hot electrons at the Pt NPs/Ti3C2 MXene interface, thereby lowering the activation barrier and accelerating the charge transfer. Overall, this work demonstrates a simple yet effective plasmon–catalyst coupling strategy that provides valuable insights for the design of next-generation plasmon-enhanced electrocatalysts for efficient hydrogen production.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yajing Zhang,Hui Wang,Zhaoyong Bian
Currently, using electrochemical precipitation techniques for phosphate removal and recovery in hydroxyapatite (HAP) or calcium phosphate (CaP) form is widely used, while the high energy consumption of electrochemical precipitation is a major obstacle to its application. In this study, a square wave pulsed electrochemical phosphate precipitation method was developed, which achieved phosphate pollution control and phosphate resource recovery and reuse at the same time. The square wave pulsed electrochemical phosphate recovery system was constructed and a Pt-rGO/CuF electrode was synthesized and evaluated. This result indicated that the Pt-rGO/CuF electrode had the highest electrocatalytic activity, the better electrical conductivity, and the smallest electron transport barrier. Under optimal operation conditions, the phosphate removal efficiency and specific energy consumption of Pt-rGO/CuF were 64.2% and 21.49 kWh kg −1 , respectively. The Pt-rGO/CuF electrode demonstrated the best electrochemical precipitation reaction performance. The Pt-rGO/CuF electrode was applied to multiple types of actual wastewater, and the results showed that it has better application prospects in both low (7.75 mg L −1 ) and high (66 mg L −1 ) phosphate concentration wastewater, the phosphate removal efficiency was 75.5% and 59.1%, respectively. Compared with traditional chemical precipitation , the electrochemical precipitation method saved $2.88 per kg P and $57.57 per kg P, respectively.
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IONICS
·
2021
·Vol. 27
·期 3
·1221-1231
·
IF 2.817
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.
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