ACS Catalysis
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2025
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IF 13.1
Xiaorui Du,Chongshuai Gao,Jiaxin Huang,Yanbin Cui,Shijun Liu,Chenguang Wang
Controlling both the hydrogenation performance and the activation of Schiff base intermediate in catalysts is crucial for attaining high slectivity toward primary amine in the reduction amination of furfural. However, it remains pending for Pt-based catalysts, on which the reduction amination reactions rarely generate primary amines so far. In this work, we developed a Pt/TiO2 nanocluster (NC) catalyst with a size distribution independent of the reduction temperature and loading amount. The reductive amination performance was investigated by regulating the surface electronic state and the distance between Pt NCs, and the results, attractively, revealed that the catalyst with a lower loading amount exhibited a higher furfurylamine (FAM) yield. Further studies unraveled that the catalyst with a larger Pt NC proximity had more abundant effective adsorption sites for the key intermediate Schiff base, i.e., the surface Ti4+ sites adjacent to the Pt NC, promoting the transformation of the Schiff base. Meanwhile, reducing the surface density of Pt NCs helped control the intensity of hydrogen spillover, thereby inhibiting the occurrence of overhydrogenation reactions. Optimal activity for primary amine generation from furfural reductive amination was achieved with a Pt NC catalyst reduced at 500 °C and with a loading amount of only 0.1 wt %, resulting in a FAM yield exceeding 93% and a production rate of 297.9 gFAM gPt h–1. The reaction mechanism, involving the competitive relationship between NH3 and H2, was elucidated through kinetic studies and theoretical calculations. This work provides insights for the designation of catalysts with controllable hydrogenation activity and adsorption selectivity and contributes to the understanding of the mechanism of the reductive amination reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Xiaolong Deng,Maolin Tian,Jian Cui,Hongtao Liu,Wenjie Zhang,Zhen Shang,Jiawei Wen,Guoyong Huang,Shengming Xu
The sustainable recovery and value-added utilisation of active metals, Pt and Re, from spent reforming catalysts represents a significant challenge in the context of industrial catalyst recycling.This study proposes an enhanced method for the selective separation and high-value utilisation of Pt and Re through the implementation of sodium roasting and weak base leaching processes.The integration of these two processes resulted in phase separation, whereby Re and Al were preferentially dissolved, while Pt was concentrated in the slag phase. Subsequent adsorption on an ion exchange resin exhibited excellent selectivity for Re/Al separation, with adsorption and desorption efficiencies of 99.67 % and 99.82 % for Re, respectively.The residual Pt was effectively recovered by oxidative acid leaching, with a combined recovery of 98.89 %.In view of the presence of trace Fe in the leach solution, the potential synergistic effect of Pt utilisation was further explored in this study. The prepared Pt/Fe@C-M intermetallic catalysts exhibited excellent electrocatalytic performance for HER, with an overpotential of 28 mV at 10 mA⋅cm −2 , which exceeded that of commercially available Pt/C catalysts.The improved performance is attributed to the beneficial electronic effect of iron in the catalyst structure. A cost-benefit analysis of the integrated recovery and value-added process was conducted, demonstrating significant commercial viability, with a net profit of $549.89 per kilogram of spent catalyst.
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MOLECULES
·
2024
·Vol. 29
·期 5
·1182
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IF 4.2
Yunqing Zhu,Kaiyue Wen,Bingqing Li,Yirong Hao,Jianjun Zhou
In this study, the performance of a zero-gap flow-through reactor with three-dimensional (3D) porous Ti/RuO2-TiO2@Pt anodes was systematically investigated for the electrocatalytic oxidation of phenolic wastewater, considering phenol and 4-nitrophenol (4-NP) as the target pollutants. The optimum parameters for the electrochemical oxidation of phenol and 4-NP were examined. For phenol degradation, at an initial concentration of 50 mg/L, initial pH of 7, NaCl concentration of 10.0 g/L, current density of 10 mA/cm2, and retention time of 30 min, the degradation efficiency achieved was 95.05%, with an energy consumption of 15.39 kWh/kg; meanwhile, for 4-NP, the degradation efficiency was 98.42% and energy consumption was 19.21 kWh/kg (at an initial concentration of 40 mg/L, initial pH of 3, NaCl concentration of 10.0 g/L, current density of 10 mA/cm2, and retention time of 30 min). The electrocatalytic oxidation of phenol and 4-NP conformed to the pseudo-first-order kinetics model, and thekvalues were 0.2562 min−1and 0.1736 min−1, respectively, which are 1.7 and 3.6-times higher than those of a conventional electrolyzer. Liquid chromatography–mass spectrometry (LC–MS) was used to verify the intermediates formed during the degradation of phenol or 4-NP and a possible degradation pathway was provided. The extremely narrow electrode distance and the flow-through configuration of the zero-gap flow-through reactor were thought to be essential for its lower energy consumption and higher mass transfer efficiency. The zero-gap flow-through reactor with a novel 3D porous Ti/RuO2-TiO2@Pt electrode is a superior alternative for the treatment of industrial wastewater.
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Catalysis Science & Technology
·
2024
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IF 4.4
Bo Ning,Zhen-Feng Huang,Chengxiang Shi,Lun Pan,Ruijie Gao,Xiangwen Zhang,Ji-Jun Zou
Commercial Pt/C is the best electrocatalyst for electrocatalytic hydrogen evolution due to its high activity and fast electron transfer kinetics. However, the poor stability under high current density and high cost limits its large-scale application. Here, we managed to fabricate a stable catalyst where MoOx stabilized Pt nanoparticles is supported on Ketjen Black via impregnation–annealing method. This catalyst exhibited a low overpotential of 4 mV (@10 mA cm−2) and 29 mV (@100 mA cm−2) and considerable long-term stability for 100 h toward acid hydrogen evolution reaction, outperforming commercial 20 wt% Pt/C. The excellent catalytic performances can be assigned to the existence of amorphous MoOx which can transport electrons to Pt nanoparticles and prevent Pt nanoparticles from agglomeration. This work provided a simple synthesis strategy to synthesize an amorphous MoOx protected Pt nanoparticles catalyst with good activity and stability, which can be an alternative to commercial Pt/C for acid hydrogen evolution reaction.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 12
·1-10
·
IF 5.3
Li Chengcheng,Lu Jinhui,Xiang Chao,Zhang Enhui,Tian Xiaofang,Zhang Ling,Li Tingting,Li Chengyao
Three-metal-core-shell nanoparticles (Au@Pt@PdNPs) providing excellent peroxidase-like activity were applied in lateral flow immunoassay (LFIA), designated as Au@Pt@Pd-LFIA, for detecting the nucleocapsid protein (NP) of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). An Au@Pt@Pd-LFIA was developed for quantitatively testing of SARS-CoV-2 NP with a range 0.12–31.25 ng/mL. The limit of detection (LOD) of Au@Pt@Pd-LFIA strip was 0.06 ng/mL, which was 16-fold or eightfold more sensitive than that of the gold lateral flow immunoassay (Au-LFIA) and the gold flower flow immunoassay (AF-LFIA) strips, respectively. For detection of clinical samples from nasal swabs using test strips, Au@Pt@Pd-LFIA had 84.09% sensitivity, 100% specificity, and 92.55% accuracy. In terms of detection time, the testing of Au@Pt@Pd-LFIA strip was 16 min similar to Au-LFIA (15 min) and AF-LFIA (10 min), but much shorter than ELISA (2 h). In conclusion, Au@Pt@Pd-LFIA is a sensitive, rapid, and simple test for quantitative detection of SARS-CoV-2 NP in nasal swab samples. Graphical Abstract
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Xiaoyan Wang,Shuangqing Sun,Meng Cheng,Lan Chen,Zhenyu Wang,Jingjie Dai
The triiodide reduction reaction (IRR) of dye-sensitized solar cells (DSSCs) and hydrogen evolution reaction (HER) of overall water splitting both face slow charge transfer, leading to lower efficiency. Herein, a multifunctional NiS 2 /Ni 9 S 8 nanocube electrocatalyst, exhibiting efficient power conversion efficiency and improved H∗ adsorption and desorption performance, is designed through sulfur ion exchange and fluorine ion etching NiCo prussian blue analog precursor. As a result, NiS 2 /Ni 9 S 8 with a matchable interface as counter electrode (CE), exhibits highly improved DSSC performance in I 3 − electrolyte, achieving a power conversion efficiency (PCE) of 9.31 %. This is mainly attributed to heterostructured interface of NiS 2 /Ni 9 S 8 , which modulates the electrons transfer from the Ni atom to I 3 − ions, activating the Ni-I bond and accelerating IRR. Additionally, NiS 2 /Ni 9 S 8 enhances HER performance in both acidic and alkaline electrolytes. Specifically, NiS 2 /Ni 9 S 8 nanocube shows low overpotentials of 117 mV and 111 mV at the current density of 10 mA cm −2 in 1 M KOH and 0.5 M H 2 SO 4 , respectively. This research develops noble-metal-free bifunctional electrocatalysts for clean and renewable energy conversion systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Shuxing Zhang,Xiaoshu Ding,Yanji Wang
5-Amino-1-pentanol is an important pharmaceutical intermediate used in the synthesis of anti-inflammatory and anticancer drugs. The direct hydrogenolysis of furfurylamine to 5-amino-1-pentanol has the advantages of a simple process route and high atom utilization. In this paper, for Pt/ZrO2 catalysts, the effects of different Pt loading and calcination temperatures on catalyst activity, selectivity, and surface properties such as Pt nanoparticle size, acidity and alkalinity, and the ratio of Pt0/(Pt0+Pt2+) were investigated. Through the study of the relationship between catalyst preparation conditions, furfurylamine hydrogenolysis reaction performance, and surface properties, it was found that moderate Pt nanoparticle size, higher Pt0/(Pt0+Pt2+) ratio, and more acidic sites favored furfurylamine hydrogenolysis. The higher number of basic sites favors the dispersion of Pt metal. The results of in situ FTIR show that the amino group of furfurylamine is adsorbed on the acidic site of Pt/ZrO2, and the furan ring is adsorbed on Pt nanoparticles, which is beneficial to the hydrogenolysis of furfurylamine.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Qian Liu,Chenye Zhang,Meimei Ren,Jinyi Wang,Leixin Feng,Yixuan Wang,Chuang Liu,Ningru Xiao,Haiming Zhang
Development of low Pt-loading electrocatalyst with enhanced activity towards oxygen reduction reaction (ORR) is highly demanded for widespread penetration of clean energy technologies. Heterointerface regulation can effectively optimize the electronic structure and intrinsic activity of the carbon supported Pt-based electrocatalyst to reduce Pt consumption. Here, by judicious choice of a sulfur-doped Fe-N-C (Fe-NS-C) as support, we construct a novel Pt/Fe-N-C heterointerface with sulfur incorporation and develop a hybrid electrocatalyst (denoted as Pt@Fe-NS-C) with ultralow Pt-loading (1.51 wt%). The incorporation of sulfur triggers the charge redistribution at the heterointerface and reduces the electron transfer from Pt to Fe-NS-C, prompting the electron density around Pt sites and boosting the electrocatalytic performance towards ORR (half-wave potential: 0.903 V; mass activity of 1.28 A mg −1 Pt at 0.9 V). In comparison, Pt species dispersed onto Fe-N-C without sulfur doping (Pt@Fe-N-C) are electron-deficient, which is not conductive to activate O 2 and results in inferior ORR activity. Zinc-air battery fabricated with Pt@Fe-NS-C as the cathode catalysts shows a large peak power density and a specific capacity of 806.7 mAh g −1 Zn . This work offers an effective way to tailor the heterointerface of hybrid or supported electrocatalyst with optimized electronic structures towards advanced electrocatalysis .
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Huangli Yan,Chengwen Yu,Xianming Zhang,Meihua Tang,Shengli Chen
The large-scale commercialization of proton exchange membrane fuel cells (PEMFCs) has been hindered by the high demand of platinum (Pt) in the cathode due to the sluggish kinetics of the oxygen reduction reaction. Reducing the amount of Pt would worsen the problems caused by the adsorption of perfluorinated sulfonic acid (PFSA) ionomers to Pt via the side chains, namely, blocking the active sites of Pt and inducing densely packed layers of fluorocarbon backbones on Pt surface to obstruct local O 2 transport at the Pt/PFSA interfaces. This work aims at optimizing the Pt/ionomer interface to mitigate the sulfonate adsorption and in the meantime to reduce the local O 2 transport resistance ( R local ), by using a porous composite of 1-butyl-3-methylimidazolium hydrogen sulfate ionic liquid (IL) modified MOF-808 (BMImHSO 4 @MOF-808) as additive in cathodic catalyst layer (CCL). Through detailed physical, spectroscopic and electrochemical characterizations, we demonstrate a three-fold optimization mechanism of Pt/ionomer interface structure by BMImHSO₄@MOF-808: the unsaturated metal sites in MOF-808 effectively inhibit the sulfonate adsorption on Pt through coordination with the sulfonates of PFSA, thereby improving catalyst utilization; the pores in MOF-808 establish efficient transport channels for gaseous oxygen, significantly reducing R local ; the IL modification layers facilitate the formation of continuous proton transport networks, increasing proton conductivity. The incorporation of BMImHSO₄@MOF-808 in a low-Pt CCL (0.1 mg Pt cm –2 ) yields a peak power density of 1.9 W cm –2 for PEMFC under H 2 -O 2 condition, and ca. 20% increase of power density under H 2 -air condition as compared with conventional CCL, indicating the prospect of IL-MOF composites as an efficient additive to enhance the performance of PEMFCs.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 8
·1-17
·
IF 5.3
Liang Jintao,Li Canru,Zhou Yu,Fan Lingling,Liu Lin,Liang Jianlu,Tan Xiaohong,Zhou Zhide,Li Guiyin
Golgi protein 73 (GP73) is highly expressed in hepatocellular carcinoma (HCC) and considered a sensitive serum biomarker for HCC diagnosis. Herein, a label-free electrochemical aptasensor for ultrasensitive detection GP73 based on nitrogen-doped reduced graphene oxide-ferrocene-platinum@palladium nanoparticles (NRGO-Fc-Pt@Pd NPs) was constructed. The NRGO-Fc-Pt@Pd NPs offered excellent conductivity, biocompatibility, and large surface area, serving as both an electrode modifier and a redox probe due to Fc's good electroactivity. GP73 aptamer (GP73 Apt ) was covalently bound with the NRGO-Fc-Pt@Pd NPs to form the signal probe. When GP73 specifically bound to GP73 Apt to form GP73-GP73 Apt complex and fell off from the electrode, it leads to an increased Fc(Fe(II)/Fe(III)) peak current in differential pulse voltammetry (DPV) due to the enhancing of the sensing interface's electroactivity. Under optimized conditions, the label-free electrochemical aptasensor demonstrated a linear relationship with GP73 concentration in the range 1.0 ng/mL-300 ng/mL, with R 2 of 0.99594 and a limit of detection (LOD) of 0.3524 ng/mL. In addition, the aptasensor showed good specificity, reproducibility, and stability. Furthermore, the developed aptasensor was applied to detect the GP73 in actual serum samples with good recoveries (97.85%-107.48%) and relative standard deviations (RSDs) (0.37%–7.85%) via the spiked recovery method. All the results may provide a new approach for HCC clinical detection. Graphical
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Jin Chen,Jiayu Lei,Jie Yan,Yuzhao Ma,Xiaofeng Yang,Yanjun Li
The establishment of a surface plasmon resonance (SPR) effect and an internal electric field (IEF) has been recognized as an effective technique for optimizing pollutant treatment in aquatic environments. Herein, we synthesized a novel 2D/2D Pt@BiOBr/Bi 2 WO 6 S-scheme heterojunction that establishes robust interfacial connections to enhance electron transport through minimized pathways, while simultaneously increasing active site availability. Subsequently, noble metal Pt was employed to modify the BiOBr/Bi 2 WO 6 composite material, thereby inducing SPR and broadening the light absorption range. Impressively, the optimized Pt@BiOBr/Bi 2 WO 6 demonstrates a significantly enhanced degradation efficiency for organic pollutants, primarily due to the synergistic effects of SPR and IEF. The degradation rate of tetracycline hydrochloride (TC-HCL) through the ternary heterojunction 2-PBB can achieve 100 % within 30 min under 500 W of visible light irradiation, showcasing impressive cyclic stability. Furthermore, the developed photocatalyst also demonstrated remarkable degradation efficiency for organic dyes such as Rhodamine B (RhB) and methyl orange (MO). This work demonstrates an original approach to the fabrication of Pt-modified S-scheme heterojunction photocatalysts with high effectiveness.
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OPTICAL MATERIALS
·
2025
·
IF 4.2
Bo Li,Yujia Liu,Lishuai Song,Yuyu Zhang,Nan Liu,Zequan Li
Absrtact This study successfully constructs a g-C 3 N 4 /TiO 2 heterojunction and its Pt nanocluster-modified composite (Pt C –CN–TiO 2 ) through an interface engineering strategy, systematically investigating their photocatalytic RhB degradation performance and mechanisms. Under visible light irradiation, Pt C –CN–TiO 2 achieves a RhB degradation efficiency of 99.29 % within 160 min, with a 34.3 % increase in reaction rate constant compared to the Pt-free catalyst. Mechanistic studies reveal that Pt acts as an electron sink, facilitating the generation of ·O 2 − , while inducing interfacial electronic structure renormalization to enhance surface hydroxyl adsorption and oxygen vacancy activity. Cycling experiments confirm its exceptional stability. This work provides novel interface engineering insights and theoretical foundations for designing highly efficient and stable solar-driven photocatalysts.
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