Interdisciplinary Materials
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2024
·
IF 24.5
Mingwei Wang,Zhiyi Hu,Jieheng Lv,Zhiwen Yin,Zhewei Xu,Jingfeng Liu,Shihao Feng,Xiaoqian Wang,Jiazhen He,Sicheng Luo,Dafu Zhao,Hang Li,Xuemin Luo,Qi Liu,Damin Liu,Baolian Su,Dongyuan Zhao,Yong Liu
Compositions and morphologies of Pt-based electrocatalysts have great impact on the electrocatalytic activity and stability of oxygen reduction reaction (ORR). Herein, we report a novel design of one-dimensional (1D) Pt–Pd dendritic nanotubular heterostructures (DTHs) by controlling the degree of Pt 2+ -Pt reduction reaction and Pd-Pt galvanic replacement reaction with uniform Pd nanowires as sacrificial templates. The obtained Pt–Pd bimetallic DTHs catalyst exhibited uniform and dense Pt dendritic nanobranches on the surface of 1D hollow Pt–Pd alloy nanotubes, possessing superior catalytic activity for ORR compared to state-of-the-art commercial Pt/C catalysts. Typically, the Pt 4 Pd DTHs catalyst showed efficient mass activity (MA, 1.05 A mg Pt −1 ) and specific activity (SA, 1.25 mA cm Pt −2 ) at 0.9 V (vs. RHE), and the catalyst exhibited high stability with 90.4% MA retention after 20 000 potential cycles. The Pt–Pd bimetallic DTHs configuration combines the advantages of 1D hollow nanostructures and dense Pt dendritic nanobranches, which results in rich electrochemical active surface sites, fast charge transport, and multiple dendritic anchoring points contact on carbon support, thus boosting its catalytic activity and stability towards electrocatalysis.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-18
·
IF 14.7
Chen Ke,Li Guo,Gong Xiaoqun,Ren Qinjuan,Wang Junying,Zhao Shuang,Liu Ling,Yan Yuxing,Liu Qingshan,Cao Yang,Ren Yaoyao,Qin Qiong,Xin Qi,Liu Shu-Lin,Yao Peiyu,Zhang Bo,Yang Jingkai,Zhao Ruoli,Li Yuan,Luo Ran,Fu Yikai,Li Yonghui,Long Wei,Zhang Shu,Dai Haitao,Liu Changlong,Zhang Jianning,Chang Jin,Mu Xiaoyu,Zhang Xiao-Dong
Strain engineering plays an important role in tuning electronic structure and improving catalytic capability of biocatalyst, but it is still challenging to modify the atomic-scale strain for specific enzyme-like reactions. Here, we systematically design Pt single atom (Pt 1 ), several Pt atoms (Pt n ) and atomically-resolved Pt clusters (Ptc) on PdAu biocatalysts to investigate the correlation between atomic strain and enzyme-like catalytic activity by experimental technology and in-depth Density Functional Theory calculations. It is found that Ptc on PdAu (Ptc-PA) with reasonable atomic strain upshifts the d -band center and exposes high potential surface, indicating the sufficient active sites to achieve superior biocatalytic performances. Besides, the Pd shell and Au core serve as storage layers providing abundant energetic charge carriers. The Ptc-PA exhibits a prominent peroxidase (POD)-like activity with the catalytic efficiency ( K cat / K m ) of 1.50 × 10 9 mM −1 min −1 , about four orders of magnitude higher than natural horseradish peroxidase (HRP), while catalase (CAT)-like and superoxide dismutase (SOD)-like activities of Ptc-PA are also comparable to those of natural enzymes. Biological experiments demonstrate that the detection limit of the Ptc-PA-based catalytic detection system exceeds that of visual inspection by 132-fold in clinical cancer diagnosis. Besides, Ptc-PA can reduce multi-organ acute inflammatory damage and mitigate oxidative stress disorder.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
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IF 8
Mengyao Qi,Yi Ke,Yifei Li,Peng Li,Huakuo Zhou,Xia Zhang,Jieshi Chen,Jun Meng
Hyaluronidase (HAase), is a naturally occurring glycosidase with the ability to break down glycosidic bonds within hyaluronic acid (HA) chains. In this paper, we propose a portable smartphone and Surface-enhanced Raman scattering (SERS) dual-mode sensor based on Au@Pt nanozyme coated with HA hydrogel to realize sensitive detection of HAase. Au@Pt nanozyme has excellent peroxidase-like activity, oxidase-like activity and catalase-like activity under acidic conditions. When HAase is present, the hydrogel structure of HA was hydrolyzed and gradually released Au@Pt nanozyme. The released Au@Pt nanozyme is used to catalyze the hydrogen peroxide system, so that 3,3′,5,5′-tetramethylbenzidine (TMB) can be oxidized into blue 3,3′,5,5′-tetramethylbenzidine (TMB ox ). Therefore, based on the above strategies, a dual-mode sensing platform for HAase detection by smartphone and SERS was established. The linear range of the dual-mode sensor platform are 2–30 U/mL and 2–80 U/mL, and the detection limits are 1.0386 U/mL and 0.004 U/mL, respectively. The dual-mode smartphone and SERS sensor platform, a combination of smartphone and Raman spectrometer, is successfully further applied to biological urine samples. This portable dual-mode sensor based on intelligent hydrogel coated nanozyme not only opens up a new way for instant detection, but also has potential applications in clinical diagnosis.
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ELECTROCHIMICA ACTA
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2012
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IF 3.832
Yang Fan,Jinhang Liu,Haiting Lu,Ping Huang,Dongli Xu
Hierarchical structure SnO 2 with two-dimensional (2D) nanosheets building blocks was employed as support material for Pt nanoparticles (NPs). The SnO 2 supported Pt catalyst was synthesized through a facile aqueous phase process using sodium borohydride as the reducing agent. The as-prepared Pt–SnO 2 catalyst exhibited remarkably improved electrocatalytic activity and stability toward methanol oxidation , in comparison with that of the commercial Pt/C catalyst and the commercial SnO 2 nanopowder supported Pt catalyst. The superior catalytic performance may arise from the unique multiscale structure and morphology of the SnO 2 support, which process extraordinary promotional effect on Pt catalyst.
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Advanced Powder Materials
·
2024
·
IF 28.6
Jingjing Yan,Rundong Wu,Guoqiang Jin,Litao Jia,Gang Feng,Xili Tong
Water electrolysis via alkaline hydrogen evolution reaction (HER) is a promising approach for large-scale production of high-purity hydrogen at a low cost, utilizing renewable and clean energy. However, the sluggish kinetics derived from the high energy barrier of water dissociation impedes seriously its practical application. Herein, a series of hybrid Pt nanoclusters/Ru nanowires (Pt/Ru NWs) catalysts are demonstrated to accelerate alkaline HER. And the optimized Pt/Ru NWs (10 % wt Pt) exhibits exceptional performance with an ultralow overpotential (24 mV at 10 mA cm −2 ), a small Tafel slope (26.3 mV dec −1 ), and long-term stability, outperforming the benchmark commercial Pt/C-JM-20 % wt catalyst. This amazing performance also occurred in the alkaline anion-exchange membrane water electrolysis devices, where it delivered a cell voltage of about 1.9 V at 1 A cm −2 and an outstanding stability (more than 100 h). The calculations have revealed such a superior performance exhibited by Pt/Ru NWs stems from the formed heterointerfaces, which significantly reduce the energy barrier of the decisive rate step of water dissociation via cooperative-action between Pt cluster and Ru substance. This work provides valuable perspectives for designing advanced materials toward alkaline HER and beyond.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xi-Lai Liu,Wei Zhong,Yu-Fan Jin,Tian-Jiao Wang,Xue Xiao,Pei Chen,Yu Chen,Xuan Ai
The electrochemical hydrogenation (ECH) of 5-hydroxymethylfurfural (HMF) to 2,5-dihydroxymethylfuran (DHMF) represents a pivotal pathway for the electrocatalytic upgrading of biomass-based organic small molecules, offering significant reductions in energy consumption while producing value-added chemicals. The conversion of HMF to DHMF is challenging due to the high reduction potential and complex intermediates of HMF ECH under neutral environment. Also, the total efficiency is hindered by sluggish anodic oxygen evolution reaction (OER) kinetics. Herein, we report a synthesis of highly alloyed Pd-Pt bimetallene (Pd 3 Pt 1 BML) for HMF ECH coupled with formic acid oxidation reaction (FAOR). Through a combination of in-situ Raman spectroscopy, electron paramagnetic resonance analysis, and theoretical calculations, we elucidate that the HMF adsorption on Pd atoms, strategically separated by Pt atoms, is weakened compared to pure Pd surfaces. Additionally, Pt atoms serve as crucial providers of active hydrogen to neighboring Pd atoms, synergistically enhancing the reaction kinetics of HMF conversion with a Faradaic efficiency >93%. Meanwhile, the atomically dispersed Pt atoms endow Pd 3 Pt 1 BML with high electrochemical performance for the direct pathway of FAOR at the anode. As a result, a FAOR-assisted HMF ECH system equipped with bifunctional Pd 3 Pt 1 BML achieves the energy-efficient conversion of HMF to DHMF at electrolysis voltage of 0.72 V at 10 mA cm –2 . This work provides insights into the rational design of bifunctional catalysts featuring two distinct types of active sites for advanced energy electrocatalysis and ECH.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Bixiao Li,Danyang Xu,Yitong Chen,Wenjing Li,Hanyu Liu,Anees A. Ansari,Ruichan Lv
How to develop antitumor nanodrugs with low toxicity and a good curative effect is an urgent problem in the current biomedicine field. In this work, different proposed composites were simulated by the finite difference time domain (FDTD) and COMSOL, including the material element, refractive index, particle size, and shape. Also, different machine learning algorithms are utilized to predict the absorbance at the near-infrared laser of 980 nm of different materials. Through train, validation, and test, the prediction of the as-synthesized Pt–Mn has high absorbance. Then, inorganic Pt–Mn was coated with PEI in order to improve their biocompatibility. Pt–Mn nanoparticles can generate ROS under the single 980 nm laser irradiation as a photodynamic therapy (PDT) agent and as a photothermal therapy (PTT) agent to heat the cells with a photothermal conversion efficiency of 23.6%. In addition, the electrochemical and in vitro chemodynamic therapy (CDT) experiments prove that Pt–Mn nanozymes could mimic the activity of peroxidase and enhance the Fenton reaction, thereby catalyzing excess H2O2 to produce hydroxyl free radicals and illustrating the potential to induce tumor cell apoptosis as the CDT agent in a weakly acidic tumor environment to complete high-efficiency chemokinetic therapy. Finally, Pt–Mn–PEI nanoparticles were used for PDT/PTT/CDT and the immune checkpoint inhibitor of anti-PD-L1 is injected in order to obtain the assistant immunotherapy, providing a potential choice to anticancer through effective synergistic cancer therapies.
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Catalysts
·
2025
·Vol. 15
·期 2
·139
·
IF 4
Yuxin Liu,Changyuan Bao,Guodong Xu,Lei Du,Bing Huang
Proton exchange membrane fuel cells (PEMFCs) have achieved milestones in performance improvements and commercial launches. In the typical commercialized PEMFCs, the compressed air to cathode is usually supplied from ambient air, assuming that no costly pre-purification system is applied. Therefore, the working PEMFCs may suffer from the negative effects of the air impurities. In this regard, SO2, as the most poisonous species, may be fed along with air at the cathode and strongly adsorbed on the Pt surface, leading to Pt site deactivation. To address this challenge, we published a series of works in terms of poisoning mechanisms, regeneration protocols, and advanced poisoning-tolerant catalysts. Herein, we are aiming at developing a SO2-tolerant electrocatalyst toward a cathodic oxygen reduction reaction (ORR). We reasonably incorporate the Ru, synthesize Ru@Pt core@shell catalysts and investigate the relationships among Ru incorporation, ORR activity and SO2tolerance. Impressively, the Ru@Pt/C exhibits higher initial ORR activity (0.288 A mg−1Pt), better SO2poisoning resistance (33% loss in initial activity) than that of commercial Pt/C catalysts (0.252 A mg−1Pt; 62% loss). The engineered affinity between Pt and SO2in the presence of Ru is uncovered to account for the improvement.
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Catalysts
·
2024
·Vol. 14
·期 4
·223
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IF 3.8
Yuhao Yang,Qiaoyun Liu,Zhongyi Liu
The catalytic conversion of naturally rich and renewable biomass into high-value chemicals is of great significance for pursuing a sustainable future and a green economy. The preparation of pentanediol from furfuryl alcohol is an important means of high-value conversion of biomass. The Pt-based catalyst supported on MgO was applied to the selective hydrogenation of biomass furfuryl alcohol to prepare pentanediol. By adjusting parameters such as catalyst loading, reduction temperature, reaction temperature, and pressure, a highly active catalyst was designed and the optimal catalytic hydrogenation conditions were determined. The hydrogenation experiment results showed that the selectivity of the 2Pt/MgO-200 catalyst for 1,2-pentanediol and 1,5-pentanediol reached 59.4% and 15.2%, respectively, under 160 °C and 1 MPa hydrogen pressure. The catalyst was characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectrometer (XPS), CO2-temperature programmed desorption (CO2-TPD), and other methods. The characterization results indicate that the reduction temperature has a significant impact on the metal Pt, and an appropriate reduction temperature is beneficial for the hydrogenation performance of the catalyst. In addition, the basic sites on the carrier are also another important factor affecting the activity of the catalyst. In addition, stability tests were conducted on the catalyst, and the reasons for catalyst deactivation were studied using methods such as thermogravimetric analysis (TGA) and Fourier transform infrared spectroscopy (FT-IR). The results showed that the activity of the catalyst decreased after five cycles, and the deactivation was due to the hydrolysis of the carrier, the increase in metal particle size, and the surface adsorption of organic matter.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xiaoyang Wang,Ziqi Fu,Ziyi Luo,Weidi Liu,Jia Ding,Jianrong Zeng,Yanan Chen,Wenbin Hu
High-loading Pt/C catalysts play an important role in the fabrication of membrane electrode assemblies with thin catalytic layer, which enhance mass transport and maintain the balance of water and heat. Unfortunately, as the loading increases, the agglomeration and growth of Pt nanoparticles (NPs) occur, causing unsatisfactory performance. Here, we present an efficient method for preparing of highly dispersed and small-sized Pt/C catalysts with Pt loadings varying from 39.01 wt% to 66.48 wt% through the high-temperature shock technique. The high density and ultrafine (~2.5 nm) Pt NPs are successfully anchored onto Vulcan XC-72R carbon black without the use of additional capping agents or surfactants. The modified carbon supports enhance the affinity for Pt precursors, contributing to loading efficiencies of 95% or more, while also providing abundant sites for the nucleation and fixation of Pt NPs, thus preventing agglomeration. In the context of the hydrogen evolution reaction in acidic media, the as-synthesized high-loading Pt/C catalysts show remarkable activity and stability, outperforming the state-of-the-art commercial Pt/C. This is mainly because the combined effects of ultrasmall and uniform Pt NPs, optimized electronic structure of Pt site, superhydrophilicity and effective anchoring of Pt NPs. The polymer electrolyte membrane electrolyzer integrated with Pt60/OX72R and commercial IrO 2 reaches 1 A cm –2 at 1.77 V and operates stably for 120 hours with a negligible voltage decay. This new strategy is fast, scalable and cost-effective for large-scale production of metal-supported catalysts, especially for the high-loading ones.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-14
·
IF 2.4
Jiang Wenjia,Zhang Pingzhu,Jia Qingqing,Zhang Zhongao,Liu Yaming,Hu Shilin,Ruan Hao,Huang Li,Wu Dong,Zhao Zhi
Hydrophobic catalysts are essential for water-hydrogen exchange reactions to facilitate the separation of hydrogen isotopes. However, existing hydrophobic catalysts are primarily small-sized pelleted forms, which are not suitable for large-scale systems. In contrast, structured catalysts, which offer a low pressure drop and enhanced mass and heat transfer properties, present promising applications. In this work, cake-like nickel foam (NF) was selected as the structural support. Activated carbon was initially loaded onto the NF using silica sol, followed by hydrothermal deposition of NiCo 2 O 4 with a rough morphology, resulting in a carrier with high roughness and a large specific surface area. The carrier attained a superhydrophobic state after modification with heptadecafluorodecyltrimethoxysilane (FD-TMS), achieving a contact angle of 163.8°. The Pt/NiCo 2 O 4 /C/NF superhydrophobic catalyst was subsequently prepared by loading Pt particles via an impregnation-gas phase reduction method. This method exposes the active metal on the surface, enhancing the Pt utilization rate. Furthermore, the extensive surface area of the carrier provided numerous attachment sites for Pt, leading to smaller particle sizes and greater exposure of Pt precursors for reduction to zero-valent Pt. The results indicated that the Pt particle size in the catalyst was 2.31 nm, with 73% of the Pt in the zero-valent form. In water-hydrogen exchange reactions, the total volume mass transfer coefficient Kya for the Pt/NiCo 2 O 4 /C/NF superhydrophobic catalyst reached 17.35 × 10 –2 s –1 , indicating strong catalytic performance. Graphical abstract
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Yong Zhang,Xin Zeng,YiYi Liu,Cuncun Wang,Changpeng Jin,Jingzhou Hou,Mei Yang,Danqun Huo
Developing an accurate, reliable, and stable glucose detection sensor poses a formidable challenge for the food industry. In this study, hydrothermal and wet chemical methods were employed to fabricate a Pt single-atom catalyst on Co3O4 (Co3O4/Pt SAs), where dispersed Pt atoms collaboratively catalyze the electrochemical reaction on the electrode surface. Subsequently, the integration of the microelectrode with polyethylene glycol diacrylate (PEG-DA) hydrogel and a dual-channel microfluidic chip facilitated continuous and rapid glucose detection. The addition of 5% PEG-DA hydrogel served to eliminate interference and expedite glucose detection, while the design of the dual-channel microfluidic chip generated microscale vortices, providing ample reaction opportunities for the target glucose while preventing interference from the mixing of previous and current reaction solutions. The research exhibited a favorable linear detection range from 1 to 800 μM, with a detection limit of 0.84 μM. Furthermore, validation of the device’s feasibility in real samples demonstrated a glucose recovery rate ranging from 94.9 to 104.4% in beverages.
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