CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ying Xu,Genkuo Nie,Xiao Jiang,Hongyu Wang,Guihua Yang,Ziyi Yan,Ji-Jun Zou,Hailong Yu,Shitao Yu,Yu Liu
Metal-metal oxide catalysts are robust in selective hydrodeoxygenation of biomass derives. Herein, 1-hexanol in total yield about 76 % is firstly achieved by high selective hydrodeoxygenation of 5-hydroxymethylfurfural over Ni/MCM-41 and Pt-WO X /t-ZrO 2 . By controlling the amount ratio of Ni/Ni 2+ to 0.46, a 99.9 % yield of 2,5-tetrahydrofurandimethanol was achieved from 5-hydroxymethylfurfural by Ni/MCM-41. Subsequently high yield of 76 % of 1-hexanol was obtained by competing pathways of tandem reactions beginning at SN2 reaction at the epoxy atom of 2,5-tetrahydrofurandimethanol to enol/tautomer intermediates and ending with controllable selective hydrogenation. The reaction mechanism is explored and the reaction-oriented regulation is realized by the additional strong BrÖnsted acid sites generated by electron transfer from W to Pt and the appropriate amount of Pt 0 sites of Pt-WO X /t-ZrO 2 , where the ratios of W 5+ /W 6+ and Pt 0 /Pt 2+ are 0.31 and 4.58 respectively. This work provides a new and green method for the synthesis of 1-hexanol and expands the utilization of metal–metal oxide in making value-added products using sustainable feedstocks.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Mingwei Zhang,Cheng-Bin Hong,Zhaoying Ding,Yujing Weng,Honghui Gong,Haiyong Wang,Yulong Zhang,Yuhe Liao,Haichao Liu
Hydrogenolysis of glycerol is an important reaction in biomass valorization, and requires efficient catalysts for selectively removing its hydroxyl groups to yield valuable chemicals, such as 1-propanol and 1,2-propanediol. In this work, we synthesized a porous and non-stoichiometric tungsten oxide (WO x ) by a solvothermal method, and a serious of WO x -supported Pt and Mn ((Mn)Pt/WO x ) catalysts by reduction with H 2 at different temperatures. On these catalysts, the product selectivity in the glycerol hydrogenolysis was significantly influenced by the presence of the Mn species and reduction temperatures. The catalysts after reduction with H 2 at lower temperatures favored the formation of 1-propanol, affording a yield of 88.0 % at 240 °C, while those reduced at higher temperatures facilitated the formation of 1,2-propanediol in a yield of 93.0 % under the same reaction conditions. Extensive analysis of these catalysts by in-situ and ex-situ characterizations showed that the high-temperature reduction led to the formation of MnWO 4 on the Mn/Pt/WO x catalysts and the consequent decrease in the acidic sites and increase in the basic sites, facilitating the alkali-assisted dehydrogenation of glycerol and selective formation of 1,2-propanediol. This study provides fundamental insights into the role of the W and Mn species in tuning the selectivity of the glycerol hydrogenolysis, which will be valuable for designing catalysts towards the valorization of other biomass-based feedstocks.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Qinyun Yan,Yanying Jing,He Xiao,Liwu Qiang,Wei Wen,Chunmei Liu,Peipei Zhao,Jiamin Ma,Shuai He,Man Zhao,Jianfeng Jia
Designing efficient electrocatalysts that synergistically optimize hydrogen evolution reaction (HER) and ethanol oxidation reaction (EOR) pathways remains a critical challenge for sustainable energy conversion. Here, we report a platinum nanocluster-anchored defect-engineered graphene catalyst (Pt/G) synthesized via exfoliation process coupled with solvothermal reduction. By modulating calcination temperature (600 °C) and KOH etching, we achieve ultrafine Pt nanoclusters (1.65 nm ± 0.39 nm) uniformly dispersed on defect-rich graphene, balancing Pt loading (0.95 wt%) and defect density (I D /I G = 0.15). The optimized Pt/G exhibits exceptional HER activity, requiring only 37 mV overpotential to deliver 10 mA cm −2 in acidic media, outperforming Pt/G-700 and Pt/G-500 counterparts. Mechanistic studies reveal that defect-mediated electronic coupling lowers hydrogen adsorption free energy (ΔG H ∗) and accelerates Volmer-Heyrovsky kinetics, yielding a Tafel slope of 26.12 mV dec −1 . For EOR, Pt/G demonstrates a mass activity of 1234.5 mA mg Pt −1 , 2.18 times higher than unetched sample. This is attributed to weakened CO intermediate binding and enhanced OH ads accessibility. Characterization results confirm that defect-rich graphene stabilizes Pt clusters against aggregation while promoting charge transfer (R ct = 27.83 Ω). This work establishes a universal strategy for engineering metal-support interactions to advance multifunctional electrocatalysts toward energy-efficient hydrogen production and biofuel utilization.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yue Tian,Zhen-Hong He,Lu-Ting Pan,Weitao Wang,Kuan Wang,Huan Wang,Hui Ma,Zhao-Tie Liu,Buxing Han
Propane-fueled solid oxide fuel cells (C 3 H 8 -SOFCs) are a promising approach for the cogeneration of light olefins (LOs) and electricity. Nickel (Ni)-based anode supports have demonstrated exceptional performance in SOFCs. However, a significant challenge arises from the propensity of C 3 H 8 to form carbon deposits. To address this, we constructed a catalytic layer composed of Ni- and Pt-doped Zn 2 TiO 4 (ZNTP) on a Ni-YSZ (yttrium-stabilized zirconia) anode. This layer catalyzes C 3 H 8 dehydrogenation to LOs and prevents direct contact between C 3 H 8 and the anode and solid electrolyte. Specifically, ZnNi alloy NPs and highly dispersed Pt atoms are formed within the catalytic layer. The ZnNi alloy enhances the electrical conductivity and oxygen vacancy concentration of the catalyst, while Pt atoms improve C 3 H 8 adsorption, providing more active sites for oxidative propane dehydrogenation to LOs. With wet 10 %C 3 H 8 -Ar (3 %H 2 O) as the anode feed, the cell delivers a LOs yield of 28.6 % at 750 °C and a peak power density of 680 mW/cm 2 , both among the highest reported for this feedstock composition. Moreover, the SOFC demonstrates remarkable resistance to carbon deposition. The work constructs an efficient dual-functional catalyst for propane dehydrogenation to LOs and offers a significant strategy for the cogeneration of valuable chemicals and electricity.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Qiuyue Ding,Huijie Wei,Yixuan Zhang,Shidong Zhao,Yanyan Xi,Songqing Hu,Xufeng Lin
Performance of the dehydrogenation catalyst is an essential issue for hydrogen storage and transportation based on liquid organic hydrogen carriers (LOHC). To overcome the problem of traditional supported noble metal catalysts, suffering from relatively low catalytic activity and selectivity, this work designed an efficient Pt–Cu synergistic catalyst by introducing additional N, O and other coordination sites as metal anchoring points in the Al 2 O 3 support during catalyst preparation. This strategy achieved high spatial isolation of Cu from Pt nanoparticles (NPs) by adding the regulator of imidazolidinyl urea to the catalytic support, actualizing highly dispersed Pt and Pt–Cu alloy nanoparticles (NPs) and subsequently quantifiable synergistic catalytic effect for dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC). Notably, the catalytic activity of Pt 2·0 Cu 0·1 /Al 2 O 3 -MR catalyst was substantially higher than that of Pt 2·1 /Al 2 O 3 -MR. A peak Pt–Cu synergistic index of 1.39 was attained in the dehydrogenation rate-determining step. The excellent synergistic effect between the Pt and Cu components was attributed to the modified electronic properties of the novel Pt–Cu alloy species under spatial confinement and the suppression of strong metal-support interactions (SMSI), as reflected by several characterization tools like XPS and HRTEM. Furthermore, the catalytic activity is also influenced by diffusion effects. DFT calculation further helped revealing that the Cu component was beneficial for the Pt cluster to lower the reaction barrier of the rate-determining step of 12H-NEC dehydrogenation.
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CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Jiale Dou,Zhuwei Yang,Linsen Li,Xinyi Hu,Li Lin,Lixia Ling,Zhao Jiang
With the global energy structure transitioning towards decarbonization, hydrogen energy has emerged as a critical energy carrier due to its merits of zero carbon emissions and high energy density. As a candidate material for liquid organic hydrogen carrier (LOHC), it is necessary to develop efficient dehydrogenation catalysts of dodecahydro-N-ethylcarbazole (12H-NECZ) to overcome the challenges of low kinetics and selectivity. In this work, by the defect engineering strategy, a series of Pt-TiO 2 catalysts are synthesized via thermal reduction using titanium (Ti) as a reducing agent. The effects of various TiO 2 :Ti molar ratios (5:1 to 8:1), annealing temperatures (550–850 °C), and Pt loadings on the structural and catalytic properties are systematically investigated. It is indicated that the 2.5Pt-7:1–650 catalyst exhibits optimal dehydrogenation efficiency, achieving 100 % conversion, 99.03 % selectivity of NECZ, and hydrogen release capacity of 5.77 wt% under 453 K and 101.325 kPa for 7 h. Various structural characterizations from XRD, H 2 -TPR, ESR, and XPS analysis reveal that the oxygen vacancies and Ti 3+ species are generated induced by the metallic Ti reduction. The interaction between Pt and TiO 2 facilitates the electron transfer from TiO 2 to Pt, optimizes the electronic state of Pt and promotes the C-H bond cleavage of benzene ring in adsorbed 12-NECZ molecules. Furthermore, the kinetic analysis for a three-step reaction pathway confirms the dehydrogenation of 4H-NECZ to NECZ is the rate-limiting step. The stability measurements suggest that 2.5Pt-7:1–650 maintains the hydrogen release amount of 5.64 wt% after 20 cycles at 453 K, demonstrating the potential applications for the NECZ/12-NECZ system. This study provides a novel strategy for designing high-performance LOHC dehydrogenation catalysts through defect engineering.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Jingxu Liu,Yanning Ren,Yi Zhao,Haoyun Zhou,Xiaohui Liu,Yong Guo,Yanqin Wang
The hydrotreatment of fats and oils for biofuel synthesis significantly contributes to carbon emission mitigation. Conventionally, this process necessitates a bifurcated pathway encompassing hydrodeoxygenation (HDO)/decarboxylation (DCO) and subsequent isomerization reactions. In this research, we synthesized a niobium-doped bifunctional catalyst, denoted as Pt/AlSiO-Nb, capable of concurrently executing HDO and isomerization of palm oil. Our examination of the palm oil hydrotreatment network, with palm acid and tripalmitin as representative model compounds, revealed that the oil undergoes hydrolysis to form fatty acids and then undergoes deoxygenation to n-alkanes via HDO or DCO routes, succeeded by n-alkane isomerization, where cracking reactions also transpire. Comprehensive characterizations of the catalyst delineated that niobium incorporation markedly augments the support–platinum interaction and proliferates the catalyst’s medium and weak acid sites, culminating in enhanced HDO and isomerization performance. These insights herald a novel methodology for biofuel generation from fats and oils, offering a streamlined approach to their catalytic transformation.
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高影响因子
BIOSENSORS & BIOELECTRONICS
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2025
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IF 10.5
Xiaobo Zhang,Xiuwen Wang,Longjiao Zhu,Jinyan Zhu,Qiuyue Zheng,Jingli Yuan,Wentao Xu,Jijuan Cao
Salmonella typhimurium ( S. typhimurium ), as common and highly pathogenic foodborne pathogen, poses a significant risk to public safety worldwide. The development of highly sensitive, rapid and on-site method for S. typhimurium analysis is urgently needed to prevent bacterial infections. Herein, we introduced a CRISPR/Cas12a-driven electrochemiluminescence (ECL) sensor based on luminol/O 2 binary systems for S. typhimurium detection, employing ultrafine Pt nanoclusters-anchored 2D delaminated-MXenes (Pt NCs/D-MXenes) as the co-reactant accelerator. The ultrathin D-MXenes support regulates the size and dispersibility of Pt NCs and facilitates the full exposure of active sites, and synergistic interactions between D-MXenes and Pt NCs improves electrocatalytic properties toward the reduction of O 2 , which promotes the generation of ROS for boosting ECL emission. Using target responsive-regulated CRISPR/Cas12a system, the ECL sensor for S. typhimurium showed a broad concentration range from 10 1 to 10 6 CFU/mL and limit of detection of 6 CFU/mL, with satisfactory recoveries in spiked-actual samples.
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
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2016
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IF 7.476
Honghong Chang,Haochun Zhang,Jia Lv,Bing Zhang,Wenlong Wei,Jingang Guo
Highly sensitive determination of tumour markers is the key for early diagnosis of cancer. Herein, triple signal amplification strategy resulting from polymer nanospheres , Pt NPs, and DNAzyme was proposed in the developed electrochemical immunosensor. First, electroactive polymer nanospheres were synthesized by infinite coordination polymerization of ferrocenedicarboxylic acid, which could generate strong electrochemical signals due to plentiful ferrocene molecules. Further, the polymer nanospheres were functionalized by Pt NPs and DNAzyme (hemin/G-quadruplex) with the ability of catalyzing H 2 O 2 , which contributes to enhance the electrochemical signals. The prepared conjugations were characterized by transmission electron microscope (TEM) and energy dispersive X-ray spectroscopy (EDX). And the process of preparation was monitored by zeta potential. Based on the sandwich-type immunoassay, the electrochemical immunosensor was constructed employing the conjugations as signal tags. Under optimal conditions, the DPV peak increased with the increasing of alpha fetal protein (AFP) concentration, and the linear range was from 0.1 pg mL −1 to 100 ng mL −1 with low detection limit of 0.086 pg mL −1 . Meanwhile, the designed immunosensor exhibited excellent selectivity and anti-interference property, good reproducibility and stability. More importantly, there were no significant differences in analyzing real clinical samples between designed immunosensor and commercial ELISA .
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Anqi Zhao,Wei Zhou,Xin Wang,Zhongjie Song,Nannan Zhang,Huan Zhang,Xinyu Gu,Jiawei Qiang,Zhengying Wu,Yong Wang,Yukou Du
Strong electronic interactions at the heterojunction interfaces of heterostructured catalysts can effectively regulate the electronic structure, optimize the adsorption of reactants and intermediates, and enhance the electrooxidation of alcohols. Due to this unique structural advantage, heterostructured catalysts are widely utilized as anode catalysts for alcohol fuel cells. However, the controlled synthesis of ternary metal heterostructures remains a significant challenge. In this study, we successfully synthesized Pt-PdPtFe ternary metal hetero-nanosheets (HNSs) using a seed-mediated method. The synergistic effects of the three metals, along with the strain effect at the heterojunction interface, contribute to the enhanced alcohol oxidation performance of Pt-PdPtFe HNSs compared to commercial Pd/C and numerous previously reported advanced catalysts. The mass activities for ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR) are 9.77 A mg Pd+Pt −1 and 6.04 A mg Pd+Pt −1 , respectively. Furthermore, CO stripping tests and durability tests indicate that Pt-PdPtFe HNSs exhibit excellent anti-poisoning ability and cyclic stability. This research presents a viable strategy for the controlled synthesis of ternary metal heterostructures, while also offering valuable insights into the rational design of high-performance electrocatalysts.
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PubMed
高影响因子
FUEL
·
2025
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IF 7.5
Shiyu Wang,Shuai Wang,Mingmei Ge,Yang Zhao,Hua Song,Huan Wang
This work introduces a template-free strategy for preparing three-dimensional (3D) honeycomb-like graphitic carbon nitride (g-C 3 N 4 ) with high specific surface area through phosphoric acid-regulated supramolecular self-assembly. By systematically tuning phosphoric acid dosage, the self-assembly process of melamine-cyanuric acid aggregates is precisely controlled, resulting in a hierarchically porous architecture with interconnected channels and abundant porosity. The optimized phosphoric acid-mediated support (SSCN-0.89) enables uniform dispersion and stabilization of ultrafine Pt nanoparticles (∼1.7 nm) via enhanced metal-support interactions. Under mild conditions (120 ℃, 0.5 MPa H 2 ), the resultant Pt/SSCN-0.89 catalyst achieves 94.1 % phenol conversion within 80 min with exclusive cyclohexanol selectivity (100 %). Mechanistic studies reveal that the hierarchical porous structure facilitates rapid mass transfer, while the tailored surface nitrogen species lower the reaction energy barrier. The catalyst retains robust stability over five cycles, demonstrating the pivotal role of 3D morphological engineering in designing high-performance carbon nitride-based catalytic supports for biomass upgrading.
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高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Jinlong Cui,Chengui Zhang,Yalong Li,Yang Liu,Weijun Jiang,Yuhui Wen,Zhenxi Wang,Zhonghua Yu,Xiangrong Ren,Zhifu Zhang
The selective hydrogenation of cinnamaldehyde (CAL) is a key reaction for producing valuable intermediates in pharmaceuticals, fragrances, and fine chemicals. However, achieving high selectivity toward the C=O bond reduction of CAL under mild conditions remains challenging. In this study, an efficient and sustainable photocatalytic strategy for the selective transfer hydrogenation of cinnamaldehyde to cinnamyl alcohol under mild conditions was reported. The low-loading 0.5 wt% Au/TiO 2 -CeO 2 and 0.5 wt% Pt/TiO 2 -CeO 2 catalysts were prepared by sol–gel and ultraviolet deposition method. Experimental results show that heterojunction is formed by doping CeO 2 with TiO 2 . The light absorption of materials is redshifted, and the separation of photogenerated electron-hole pairs is enhanced, thereby reducing the load usage of precious metal. The 0.5 wt% Au/TiO 2 -CeO 2 catalyst exhibits optimal performance under visible light irradiation, while the 0.5 wt% Pt/TiO 2 -CeO 2 catalyst exhibits excellent activity under ultraviolet light irradiation. The conversion efficiency in 0.5 wt% Au/TiO 2 -CeO 2 catalytic system under visible light is 97.23 %, and the selectivity can reach 96.91 %. Recycling tests verified the structural stability and reusability of the prepared catalysts. The formation of heterojunction structures can effectively reduce the load of precious metal while maintaining high conversion and selectivity. These findings provide a new pathway for achieving highly selective CAL hydrogenation under mild conditions.
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高影响因子
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