Fundamental Research
·
2025
·
IF 6.3
Zhong Wang,Tuo Zang,Ye Ziyu,Siyuan Zhang,Guojian Li,Xiaoming Liu,Qiang Wang,Shuang Yuan
Precise anchoring and high-density utilization of platinum single atoms (Pt SA ) remain critical challenges in advancing efficient hydrogen production via water electrolysis. Here, we present an innovative magnetic-field-assisted electrodeposition strategy for the controllable synthesis of high-density Pt SA on two-dimensional MXene substrates. Application of a 0.6 T magnetic field significantly enhanced Pt SA deposition kinetics, yielding a 2.1-fold increase in the deposition rate. Numerical simulations confirmed that magnetohydrodynamic (MHD) effects induced by the magnetic field were the primary mechanism driving this enhanced deposition efficiency. The optimized Pt SA -0.6@MXene/NF catalyst exhibited outstanding hydrogen evolution reaction (HER) performance in 1 M KOH, achieving an ultralow overpotential of 12 mV at 10 mA cm −2 , along with a Tafel slope of 29 mV dec −1 . Notably, the catalyst demonstrated 66.1-fold higher Pt mass activity (3458.7 A g −1 ) compared to commercial Pt/C (52.3 A g −1 ) at a 50 mV overpotential. Density functional theory (DFT) calculations revealed that the high-density Pt SA configuration synergistically enhances MXene's electrical conductivity while lowering the d-band center, thereby optimizing the energy barrier for hydrogen intermediate (H*) adsorption. This work provides a novel strategy for regulating the magnetic-field-assisted deposition of Pt SA catalysts, offering a new avenue for designing high-performance water electrolysis catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Zhuo Wang,Meiting Wang,Luan Fang,Zihan Li,Ping Nie,Yuting Gao,Juan Jian,Limin Chang
Hydrogen produced through self-powered water-splitting can effectively meet the demand for miniaturized devices. However, the design of an efficient catalyst that integrates a zinc-air battery (ZAB) with a water-splitting cell is crucial for the development of such devices. In this study, we synthesized Pt/Ni 3 (PO 4 ) 2 on nickel foam (NF) via a two-step process. The resulting Pt/Ni 3 (PO 4 ) 2 /NF exhibited significantly enhanced trifunctional properties (hydrogen evolution reaction, HER; oxygen evolution reaction, OER; oxygen reduction reaction, ORR) compared to the Ni 3 (PO 4 ) 2 /NF precursor. Additionally, the ZAB assembled using Pt/Ni 3 (PO 4 ) 2 /NF as the air-cathode demonstrated superior rechargeable performance compared to the Ni 3 (PO 4 ) 2 /NF-based counterpart. Moreover, when Pt/Ni 3 (PO 4 ) 2 /NF was directly used as both the cathode/anode for the water-splitting device and the air-cathode for the ZAB, the self-powered hydrolysis device exhibited excellent hydrogen production performance. Upon investigating the influence of in-situ decorated Pt nanoparticles, we found that these Pt nanoparticles: 1) facilitate the morphological reconstruction of Ni 3 (PO 4 ) 2 , thus increasing the electrochemical surface area of the catalyst; 2) lower the hydrogen adsorption free energy of Pt/Ni 3 (PO 4 ) 2 , and the associated OER theorical potential; 3) shift the d-band center of Pt/Ni 3 (PO 4 ) 2 closer to the Fermi level, ultimately enhancing its intrinsic catalytic activity. This work is expected to provide a foundation for experimental, theoretical, and practical applications of other Ni 3 (PO 4 ) 2 -based multifunctional materials.
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CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Jiale Han,Guofan Wang,Xu Hu,Jinlin Li,Zhaojun Xie,Zhen Zhou
Rechargeable lithium oxygen (Li–O2) batteries are regarded as promising candidates for future energy storage systems due to their exceptionally high theoretical energy density. However, their practical implementation faces major obstacles, including high charge and discharge overpotentials and a semiopen battery structure that is highly sensitive to humidity. These factors lead to reduced efficiency and poor stability in moist air, significantly limiting real-world application. To address these challenges, a composite photoelectrode was developed by directly growing tungsten trioxide (WO3) nanoribbons on carbon paper (CP), followed by the uniform deposition of platinum nanoparticles using atomic layer deposition. Compared to WO3 photoelectrode, the resulting Pt–WO3 photoelectrode enables stable operation of photoassisted Li–O2 batteries under humid oxygen atmosphere. The batteries sustain stable operation for over 100 cycles without failure at current densities of 0.05 and 0.2 mA cm–2. Advanced characterization and theoretical calculations confirm the formation of an ohmic contact between platinum and tungsten trioxide, which promotes the separation of photogenerated electrons and holes, improves charge transfer, and facilitates the reversible formation and decomposition of lithium hydroxide (LiOH). This strategy effectively overcomes critical barriers faced by conventional Li–O2 batteries in real-world environments and provides a promising direction for the design of environmentally tolerant and photoelectrochemically efficient energy storage systems.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Chao Wang,Hu Zang,Changjiang Liu,Jiahao Wang,Long Kuai,Baoyou Geng
The hydrogen evolution reaction (HER) involves two-step elementary reactions, providing an opportunity to establish dual-site synergistic catalysts. This work demonstrates carbon-supported Pt single atoms and clusters (Pt1+Cs-NPC) as an efficient catalyst for acidic HER, which exhibits an ultralow Tafel slope of 12.5 mV/dec and an overpotential of 24 mV at 10 mA/cm2 with an ultralow platinum content of 3.8 wt %. The Pt mass activity and turnover frequency (TOF) are 10.2 times and 5.4 times that of commercial Pt/C, respectively. The density functional theory (DFT) study shows that the Pt cluster regulates the electronic state structure of the adjacent Pt single atom, so that the ΔGH* at the Pt1 site approaches 0. Moreover, the DFT study confirms that Pt clusters and neighboring Pt single atoms can synergistically catalyze the Tafel step and reduce the energy barrier in forming the H–H bond. At the same time, the platinum cluster reduces the energy barrier of the nearby platinum single-atom site to the Heyrovsky step and accelerates the reaction with hydrated hydrogen ions. Studies have shown that platinum clusters and platinum single-atom composite loading structures exhibit excellent activity for the Volmer–Tafel or Volmer–Heyrovsky reaction paths of HER reactions. This work provides a clear understanding of the synergistic effect of Pt1+Cs-NPC, which provides guidance for developing efficient HER catalysts.
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Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 38
·11880-11886
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IF 0
Xianguang Ding,Yu Zou,Feng Ye,Jun Yang,Jiang Jiang
Hybrid nanostructures can combine two or more functionalities in one unit and oftentimes exhibit synergistically enhanced properties compared to the simple sum of the constituents. Herein, we demonstrate the facile synthesis of Pt–CuS heterogeneous nanoparticle dimers based on the sulfidation of the corresponding bimetallic alloy templates. It begins with the preparation of CuPt alloy nanoparticles in an organic solvent, which are then converted into Pt–CuS heterodimers by reacting with elemental sulfur in octadecene at elevated temperatures. The Pt–CuS heterodimers display highly selective activity for catalyzing the methanol oxidation reaction at room temperature due to the strong electronic coupling effect between the different domains in the heterodimers. The structural transformation from alloy to heterogeneous nanomaterials may provide new opportunities to design and fabricate hybrid nanostructures with interesting physicochemical properties.
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RSC Advances
·
2022
·Vol. 12
·期 34
·22070-22081
·
IF 4.036
Xin Fu,Ruisong Li,Yucang Zhang
This study explores an aerosol-assisted method to prepare an efficient support for the Pt catalyst of polymer electrolyte membrane fuel cells (PEMFCs). Titania nanoparticles and mesoporous niobium-doped titania nanoparticles were prepared by aerosol-assisted self-assembly using titanium(IV) isopropoxide and niobium(V) ethoxide as the titanium and niobium sources for application as non-carbon supports for the platinum electrocatalyst. The structural characteristics and electrochemical properties of the supports were investigated by transmission electron microscopy, X-ray diffraction, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, inductively coupled plasma optical emission spectrometry, and dynamic light scattering. The Brunauer–Emmett–Teller method was used to calculate the specific surface areas of the samples, and the pore size distribution was also examined. The results demonstrated that under a radial concentration gradient, the aerosol droplets self-assembled into a spherical shape, and mesoporous supports were obtained after subsequent removal of the surfactant cetyltrimethylammonium bromide by annealing and washing. The hydrothermal technique was then used to deposit platinum on the TiO2-based supports. The electrical conductivity of the non-carbon support was enhanced by the strong metal–support interaction effect between the platinum catalyst particles and the porous niobium-doped TiO2 support. The half-wave potential, electrochemical surface area, mass activity, and specific activity of the obtained Pt/Nb-TiO2 catalyst all surpassed those of commercial Pt/C.
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Journal of Environmental Chemical Engineering
·
2019
·
IF 0
Limei Cao,Qian Wang,Ji Yang
A novel ultrafine Pt/Beta catalyst supported on carbon paper was prepared and applied to selective catalytic reduction of NO x by H 2 at a low temperature below 90 °C. Here, 0.8 wt.% Pt/Beta reached approximately 100 % NO conversion at 90 °C under oxygen-rich conditions (1000 ppm NO, 1 % H 2 , and 4 % O 2 ). The influence of the dispersion and particle size of Pt on the catalytic performance was investigated using Polyvinylpyrrolidone (PVP) as a structure directing agent to regulate the Pt particles. The feeding amount of PVP significantly influenced the catalytic activity of the catalysts. When the feeding amount was less than 50 mg, the Pt particle size was smaller, and the dispersion was higher, providing a higher NO conversion. However, when the feeding amount exceeded 50 mg, the dispersion no longer increased, and the activity slightly decreased. N 2 physisorption (BET) confirmed that excessive PVP decreased the specific surface area, which suppressed the catalytic activity of Pt/Beta. Moreover, the NO conversion efficiency was dependent on the dispersion and particle size of Pt and was minimally affected by the surface area of the catalysts. The Pt/Beta catalyst system was deactivated, and an irreversible poisoning phenomenon for SO 2 was observed. Zr, Ce, and V were introduced into the catalyst system as metal auxiliaries . The Ce-modified Pt-Ce/Beta catalyst prepared in this study showed resistance to SO 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Changchun Sun,Chao Wang,Guangting Han,Yuanming Zhang,Haiguang Zhao
The application of layered molybdenum disulfide (MoS 2 ) in catalytic hydrogen production has attracted great interest, while their catalytic properties are limited by poor electron conductivity and a few catalytically active sites. In this work, we demonstrated a highly active electrocatalyst for large-scale hydrogen production, consisting of two-dimensional (2D) Pt-MoS 2 nanosheets along one-dimensional (1D) cobalt nanoparticle integrated carbon hollow nanofibers (Co@CHNF). The as-prepared Pt-MoS 2 -Co@CHNF had a large specific surface area (44.5 m 2 g −1 ). X-ray photoelectron spectrometer (XPS) and spherical aberration corrected transmission electron microscope (AC-STEM) demonstrated that Pt atomic clusters (Pt ACs) were doped on MoS 2 nanosheets by thermodynamically induced spontaneous interfacial redox between MoS 2 and H₂PtCl₆. The Pt-MoS 2 -Co@CHNF based catalysts exhibited an overpotential as low as 91 mV for 10 mA cm −2 and 258 mV for 200 mA cm −2 in 1 M KOH electrolyte, and there is no significant floating for catalytic active with 14 h continuous operation, which demonstrates its excellent long-term operation durability, significantly superior to the previously reported state-of-the-art Co-based or Mo-based catalysts. In particular, the self-supporting binder-free Pt-MoS 2 -Co@CHNF catalyst-based electrode showed an ultra-high current density of 500 mA cm −2 at a low overpotential of 301 mV, without any decrease after 24 h operation at 500 mA cm −2 in 1 M KOH seawater electrolyte, representing a great potential for large-scale seawater hydrogen production.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Chaohui Guan,Jiefei Li,Tao Chen,Liang Lv,Junfeng Du,Shuai Zhang,Hang Wei,Haibin Chu
Developing high performance catalytic materials for the electro-oxidation of glycerol into specific value-added products is essential for glycerol valorization. Herein, we used the sol–gel method to coat the TiO2 layer with adjustable thickness on the surface of carbon nanotubes (CNTs), obtaining a unique morphology of porous sheath TiO2 wrapped CNTs (TiO2/CNTs). Subsequently, Pt nanoparticles were loaded onto TiO2/CNTs using the ethylene glycol reduction method. The prepared Pt–TiO2/CNTs catalyst achieves a glycerol conversion near 100% at 0.8 V vs. RHE and 60 °C for 10 h. Notably, the selectivity of tartronate reaches 52.5% after 24 h. Characterization results reveal that the dispersed Pt nanoparticles are embedded into the holes of the TiO2 porous sheath, fabricating abundant Pt–TiO2–CNT interface structures. The infusion of TiO2 shifts the center of the d-band upwards, and enhances the adsorption of the glycerate intermediate on Pt particles, which facilitates the further oxidation of glycerate to tartronate. This simple and efficient morphology control method provides a new strategy for glycerol valorization via electrocatalysis.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Chen Yuanxing,Qin Ying,Liu Mingwang,Yang Wenhong,Qiu Yiwei,Li Wen,Zheng Lirong,Gu Wenling,Zhu Chengzhou,Hu Liuyong
Energy level mismatches between semiconductors and cocatalysts often induce carrier recombination, limiting photocatalytic and photoelectrochemical (PEC) efficiency. Here, we integrate Pt nanocluster-Fe single-atom pairs with CuO to regulate both solid-solid and solid-liquid interfaces in PEC systems. Experimental and theoretical analyses reveal that an Ohmic contact at the CuO/Pt interface accelerates electron extraction, while Pt-to-Fe charge transfer enhances oxygen reduction at Fe sites, collectively boosting reaction kinetics. Leveraging this, we construct a PEC biosensor exploiting chelating effect of glyphosate on CuO to impede electron transfer, achieving a detection limit of 0.41 ng/mL. This interface engineering strategy advances cocatalyst design for enhanced energy conversion and sensing applications by simultaneously addressing carrier dynamics and interfacial reaction barriers.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiangyun Xiao,Yiming Shang,Yang Bai,Han Miao,Xiaowang Lu,KyuJoon Lee,Jae-Pyoung Ahn,Osama Younis,Taekyung Yu,Xinchun Yang
Efficient and stable catalysts are crucial for green hydrogen production from acidic water splitting. Herein, using interface engineering, the surface electronic structures of bimetallic PdRu nanocubes have been significantly regulated by Pt atoms (PdRu@Pt). Interestingly, Pt atoms are located on the corners and facets of PdRu nanocubes, resulting in lattice tension and fast electron transfer . As a result, the obtained trimetallic PdRu@Pt nanocubes with an average size of 13 nm have exhibited highly enhanced catalytic activity and stability for hydrogen evolution reaction (HER) in acidic media, delivering 18 mV lower overpotential to reach a current density of 10 mA cm −2 , and maintaining a remarkable long-term stability for up to 24 h. In particular, the lower overpotential of 489 mV at 500 mA cm −2 for PdRu 0.04 @Pt 0.12 nanocubes indicates its potential for future industrial application in the future. Such enhancements in HER performance can be attributed to the highly facet-edge-exposed Pt atoms and the significant strain effects resulting from the introducing Pt atomic layers to PdRu surfaces.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Yining Dong,Ping Song,Ce Han,Weilin Xu
In this paper, Pt-Fe alloy with low-content of Pt (2 %) was distributed uniformly over the porous Fe/NC substrate treated by nitric acid etching, with small amount of metallic Fe and Pt nanoparticles. The optimized Pt-Fe alloy on Fe/NC substrate showed higher ORR performance with the E 1/2 of around 0.83 V vs. RHE as well as faster catalytic kinetics. In addition, the catalytic activity has not been decayed through an accelerated durability test after 5000 cycles CVs, indicating better catalytic stability for the alloying catalyst. The introduction of Pt elements into Fe/NC substrate increased the numbers and species of ORR active sites, invoking higher ORR activity comparing with isolated Fe/NC catalyst. The acid etching provided more defects for the substrate to anchor the active sites stably. Moreover, the synergistic effect originated from the alloying of Pt and Fe modulated the electronic structure of Pt, increasing the ORR activity with low yield of H 2 O 2 . This decreasing H 2 O 2 yield can weaken the Fenton reaction to prevent the dissolution of Fe in the acid solution, which can improve the stability of the catalysts to meet the commercial needs for PEMFC.
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