JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Chengfeng Wang,Hongdong Li,Weiping Xiao,Zhenyu Xiao,Guangrui Xu,Dehong Chen,Zexing Wu,Lei Wang
The interaction between metal nanoclusters and the carrier can enhance the electron transfer rate to optimize the hydrogen evolution reaction (HER) performance, but the common synthesis approaches often lead to metal particle agglomeration, and then blocking active sites. Herein, highly-dispersed Pt nanoclusters supported onto molybdenum boride (MoB) is developed through microwave approach with various solvent to regulate the catalytic performance. The synthesized electrocatalyst with the addition of methanol (Pt/MoB-M) exhibits excellent electrocatalytic performance towards HER with low overpotential (13 mV at 10 mA cm −2 ), small Tafel slope (24 mV dec −1 ), and high mass activity (10.06 A/mg Pt at 50 mV). This work presents a novel approach to prepare highly-efficient electrocatalysts for renewable energy-related applications of non-carbon supported low loading of precious metals.
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ChemCatChem
·
2024
·
IF 3.8
Huan Yang,Xu Wang,Haowei Wang,Ya-Dong Xie,An-Hui Lu
Graphical The Sn species doped by coprecipitation with Al precursor introduces additional acidic sites on Sn-doped alumina, which after loading with Pt species exhibits superior reactivity and stability for propane dehydrogenation. Alumina-supported PtSn catalysts have been industrialized as the major catalysts for propane dehydrogenation, where Sn serves as an essential promoter. Herein, we synthesized a variety of Sn-doped alumina supports by regulating the precipitation order of Sn and Al precursors as follows: Sn precursor precipitated before Al, coprecipitated with Al, precipitated immediately after Al, or precipitates after 2 h of Al. The effect of Sn promoter on the surface acidic properties of alumina and, ultimately, on propane dehydrogenation was further investigated. The Sn species introduced by coprecipitation in alumina created additional surface strong acid sites, attributed to more Sn 4+ species on the surface, which are able to remain stable during the subsequent treatment. Consequently, the coprecipitated Sn species in the corresponding catalyst donate more electrons to Pt and reduce the metal particle size. As a result, the catalyst with Pt supported on the coprecipitated support (Sn+Al) exhibits superior initial propane conversion (43.2%) and stability ( k d = 0.035 h −1 ). This study provides new insight into the interaction between the two key components, tin promoter and alumina support, of Pt/Sn-Al 2 O 3 catalysts.
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POLYMER DEGRADATION AND STABILITY
·
2024
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IF 6.3
Dingsong Wang,Wanyan Li,Jingjing Qin,Youwei Zhu,Liyan Liang,Changan Xu
Liquid silicone rubber (LSR) exhibits excellent thermal stability and has been selected for use in a variety of applications where thermal stability, chemical resistance and fire-retardant are required. The enhancement of the organic-to-inorganic conversion of LSR to improve their flame-retardant properties represents a significant area of research. The thermal stability of the platinum catalysts and the crosslinked network structure of the LSR have a considerable influence on the organic-to-organic conversion behavior of LSR. The present study demonstrates the efficacy of N-heterocyclic carbene (NHC) ligand-modified Karstedt's catalysts as catalysts for the curing of LSR by hydrosilylation at room temperature and for the organic-to-inorganic conversion of LSR at elevated temperatures. The catalyst was employed in the preparation of three LSRs with varying network structures, utilizing four polysiloxanes with differing degrees of functionality. The pyrolytic behavior and organic-to-organic conversion rate of these LSRs were investigated using a thermogravimetric analyzer (TG) coupled with a Fourier transform infrared spectrometer (FTIR). The findings indicated that LSRs with the highest crosslink density exhibited the highest organic-to-inorganic conversion rate; however, they demonstrated the lowest fire-resistance. The anomalous behavior has been subjected to further analysis with respect to the mechanical properties of the LSRs and the characteristics of their network structure. LSR coatings with enhanced hardness and fire-resistance are then produced by combining the advantageous properties of both LSRs in a layer-by-layer (LBL) assembly.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zhiyin Huang,Yuqin Peng,Lixin Xing,Mijia Xu,Meng Fang,Huiqi Xie,Jiamin Li,Yangdong Zhou,Puwei Wu,Ning Wang,Chunmei Tang,Mingjie Wu,Liguang Wang,Siyu Ye,Lei Du
Platinum (Pt) is inevitably employed to facilitate various electrocatalysis including hydrogen oxidation/evolution and oxygen reduction reactions (HOR/HER/ORR), the foundation for renewable energy conversion and storage. Pt-based high-entropy-alloy (HEA) catalysts have been recently presenting promises to improve intrinsic activity of unit mass Pt. However, their current synthesis methods always produce large particles—some can control small size but have to use complicated recipe and/or highly toxic and expensive chemicals. Alternatively, a facile microenvironment regulation strategy is herein proposed to tune solvent polarity and nanoparticle-support interactions within the precursors for carbon-thermal shock pyrolysis. We found that the decreased solvent polarity and enhanced particle-support affinity can jointly control the nanoparticle size ultimately to ∼2.68 nm with ∼10 wt% Pt loading. The compressed lattice fringe in such HEA particles leads to electron accumulation at Pt atoms and build a moderate charge density rearrangement, showing superior multifunctional HER/HOR/ORR activity to Pt/C in acidic media.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
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IF 8
Fangfang Yang,Shuang Li,Xiaolin Zhang,Li Wang,Shufeng Liu
Herein, biomodification-free Pt nanoparticles (Pt NPs) were directly employed to construct new single-particle collision electrochemical biosensors, which were based on rational control of sulfhydryl group onto the magnetic beads (MBs) surface for Pt NPs capture. As proof of concept, human immunodeficiency virus DNA (HIV-DNA) was chosen as a model target. The hairpin-like DNA probes were conjugated onto the MBs and the sulfhydryl groups labeled at the end of hairpins were confined onto the MBs. The target recognition induced the exposure of the caged sulfhydryl groups for efficient capture of Pt NPs and polymerase-powered target recycling contributed for signal amplification. After magnetic separation, the amount of freely diffusing Pt NPs in solution for electrocatalytic hydrazine oxidation decreased, resulting in target-dependent collision frequency change. With the developed sensing mode, the sensitive detection of target DNA with a low detection limit of 0.13 pM could be achieved. It also demonstrated a good detection selectivity toward other nucleotide sequences and could be applied for target detection in serum system. An extended application of current collision-based sensing mode for protein kinase (PKA) activity was also proposed, which was based on PKA-catalyzed peptide phosphorylation to introduce new sulfhydryl groups onto MBs for Pt NPs capture. By monitoring the changes in the collision of Pt NPs, the activity of PKA and its inhibitor were well determined. Thus, this work provides new avenue toward the development of single-particle collision-based biosensors for highly sensitive and accurate bioanalysis by integrating specific biorecognition and/or amplification process and biomodification-free nanoparticles.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Hao Zhu,Yang Wang,Xiaoling Zheng,Pan Li,Yingying Zhu,Xinbao Li
Green hydrogen production from renewable biomass via bio-oil catalytic steam reforming was a prospective technology. In order to accelerate the development of high-performance and long-term catalyst, we selected acetic acid as a typical bio-oil model compound to carry out the studies of steam reforming. Excellent bimetallic Pt-Co/Al 2 O 3 catalysts were prepared using a sol-gel auto-combustion method. The effects of the molar ratio of ethylene glycol : citric acid : metal ions (EG/CA/M) on the catalyst structure and subsequent reforming performance were systematically investigated. It was found that the catalyst’s textural properties, reducibility , basic sites, and the dispersion of active metal could be carefully tuned by the EG/CA/M ratio. The catalyst prepared under EG/CA/M ratio of 6:3:1 performed the best reactivity in acetic acid steam reforming, showing a 97.6% acetic acid conversion and a 96.6% H 2 yield at the reaction conditions of 650 °C, steam to carbon molar ratio of 5, and space velocity of 6957 h –1 . Furthermore, a bifunctional reaction mechanism of acetic acid catalytic steam reforming was proposed by in-situ diffuse reflective infrared Fourier transform spectroscopy analysis coupled with density functional theory calculations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaofeng Wang,Yangping Zhang,Tianpeng Liu,Zhengying Wu,Jun Yu,Yukou Du
Zeolitic imidazolate frameworks (ZIFs), a class of promising metal organic frameworks (MOFs) material, display high porosity and chemical/thermal stability. However, there are problems such as few active sites and restricted exposed active areas, which limit the oxygen evolution reaction (OER) performance of catalysts. Here, starting from zeolitic imidazolate framework-67 (ZIF-67), we have successfully synthesized Pt-doped CoFe layered double hydroxide (Pt/CoFe LDH) catalysts for efficient OER catalysis. The obtained Pt/CoFe LDH-4 catalysts provides large surface areas and abundant active sites, which further improves the OER performance. In detail, the Pt/CoFe LDH-4 exhibits a lower overpotential of 263 mV at a current density of 40 mA cm −2 , in 1 M KOH solution, the stability of the catalyst exceeds 120 h at this current density, far superior to commercial catalyst RuO 2 . This study describes a new design idea for synthesis of LDH catalytic materials with low noble metal doping, which broadens the way to the synthesis of robust OER catalysts derived from ZIF-67.
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Reaction Chemistry & Engineering
·
2024
·
IF 3.4
Yongming Xu,Wenzhao Liu,Bo Xu,Ke Wang,Jinchu Yang,Yueqi Si,Xuebin Zhao,Tingting Zhang,Zhan Zhang,Xueyi Qiao,Tianliang Lu
Glycolic acid finds extensive applications in the production of biodegradable polymers, pharmaceuticals, and fine chemicals. In this study, a Pt catalyst supported on the Sn-Beta zeolite (Pt/Sn-Beta) was developed to achieve the efficient and highly selective catalytic oxidation of ethylene glycol with molecular oxygen to prepare glycolic acid at near-room temperature (30 °C). Characterization results, including XRD, TEM, XPS, FT-IR, and O2-TPD, revealed that the relatively uniform dispersion of Pt particles, the optimal density of Lewis and Brønsted acid sites in the catalyst, and the synergistic interaction between Sn and Pt sites might be key factors contributing to the excellent catalytic performance of the Pt/Sn-Beta catalyst. By optimizing the reaction conditions, a 90% conversion of ethylene glycol and an 81% selectivity of glycolic acid were obtained. Furthermore, Pt/Sn-Beta exhibited excellent stability, with no significant decrease in catalytic performance after six repeated uses.
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International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 9
·2260-2269
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IF 7.2
Xie Zhipeng,Zhang Da,Peng Haiyang,Lei Yong,Yang Bin,Liang Feng
Nitrogen-doped single-walled carbon nanohorns (N-SWCNHs) can serve as an effective carrier for platinum (Pt) catalysts, which has the potential to improve the electrocatalytic activity of oxygen reduction reaction (ORR) and the operation life of the catalyst. In this work, dahlia-like SWCNHs with N contents ranging from 2.1at% to 4.3at% are controllably synthesized via arc discharge and applied as a carrier of Pt nanoparticles (NPs), denoted as Pt/N-SWCNHs. Pt/N-SWCNHs-2:1 (graphite and melamine with the mass ratio of 2:1) exhibits excellent electrocatalytic activity (onset potential = 0.95 V). The half-wave potential of Pt/N-SWCNHs-2:1 is only reduced by 2 mV after 3000 cyclic voltammetry cycles. This can be attributed to the enhanced dispersion of Pt NPs and the strong electronic interaction between the N-SWCNHs and Pt, facilitated by the optimal nitrogen doping level. The results of this work offer important perspectives on the design and enhancement of Pt-based electrocatalysts for ORR applications, highlighting the critical role of the nitrogen doping level in balancing the electrocatalytic activity and long-term stability.
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ACS Catalysis
·
2025
·
IF 13.1
Bo Tang,Xu Zuo,Ang Li,Jiajun Wang,Haojun Zou,Lili Xu,Weili Dai
Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., AuxPty@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au1Pt3@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h–1 at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O2 and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.
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Journal of Magnesium and Alloys
·
2025
·
IF 13.8
Guorong Zhang,Taigen Liang,Fen Xu,Lixian Sun,Sheng Wei,Jiaxi Liu,Lina Qin,Xia Lin,Yongpeng Xia
Magnesium hydride (MgH 2 ) is a promising solid-state hydrogen storage material due to its high hydrogen content and cyclic stability. However, its practical applications are limited by slow desorption kinetics and a high dehydrogenation temperature. To address these challenges, Pt-loaded MAX fibers with oxygen vacancies (Pt@MFs) have been synthesized by using vortex and hydrothermal methods. And the effects of the Pt@MFs on the hydrogen storage properties of MgH 2 are investigated. The results display that the MgH 2 doped with 10wt% Pt@MFs begins dehydrogenation at 169.3 °C and absorbs 5.73 wt% hydrogen in just 30 s at 125 °C and 30 bar hydrogen pressure. After 30 cycles, the MgH 2 –10 wt% Pt@MFs retains 98.7% of its initial capacity, showcasing excellent cycling stability. The synergistic effect of the MAX fiber network's active sites, oxygen vacancies, anchored Pt nanoparticles and intermetallic compounds (PtTi, Pt 3 Ti) in the MgH 2 –10 wt% Pt@MFs composite significantly enhances hydrogen storage kinetics by facilitating diffusion, optimizing electron transfer, and weakening Mg-H bonds. The design concept of this material offers a novel strategy for improving the kinetics and stability of MgH 2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shenghang Peng,Rong Li,Jing Li,Jian-Ping Zou,Alex Aziz,Xuxing Chen
Effective removal of ethylene (C 2 H 4 ) during fruit and vegetables storage and transport remains a critical challenge for post-harvest preservation. Although S-scheme heterojunctions can improve charge separation and redox capacity for ethylene degradation, their efficiency is still restricted by limited carrier transfer and sluggish oxygen activation. Here, we rationally designed a novel 2D/2D SnNb 2 O 6 /Bi 2 MoO 6 monolayer S-scheme heterojunction integrated with Pt co-catalyst to address these limitations. Density Functional Theory (DFT) calculations revealed the S-scheme charge transfer pathway, which was experimentally realized via electrostatic self-assembly followed by annealing-induced atomic interface bonding. Photodeposited Pt nanoparticles further promoted O 2 activation at reduction sites. The optimized Pt-50-SNOBMO achieved an outstanding visible-light-driven degradation rate (139.2 × 10 −3 min −1 ), 248.6 and 143.5 times higher than pristine SnNb 2 O 6 and Bi 2 MoO 6 , representing the best performance reported to date for ethylene removal. Extensive spectroscopic and microscopic analyses confirmed the robust interface interactions and S-scheme mechanism. This study provides new insights into heterojunction engineering and offers a promising strategy for advanced photocatalytic preservation technologies.
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