ACS Applied Energy Materials
·
2025
·
IF 5.5
Henan Shang,Qi Jia,Sijia Li,Jinsheng Liang
The rational design of efficient and selective catalysts for formic acid (FA) dehydrogenation is critical yet challenging for the development of hydrogen-based energy applications. Herein, ultrafine trimetallic NiAuPd nanoparticles (∼1.65 nm) supported on nitrogen–phosphorus-doped graphene (NPG) with excellent dispersibility have been successfully prepared. Remarkably, the optimized Ni0.2Au0.2Pd0.6/NPG catalyst exhibits exceptional catalytic activity and robust stability for additive-free FA dehydrogenation at 303 K, achieving 100% hydrogen selectivity and an unprecedented initial turnover frequency (TOF) of 10053.96 mol of Pd–1 h–1. The significant enhancement in catalytic activity can be attributed to the synergistic effects, including the optimized electronic structure and improved electron transfer facilitated by Ni incorporation, the precise control of particle size and dispersion by NPG support, and the strong metal–support interaction (SMSI) between the NiAuPd nanoparticles and the NPG substrate. Density functional theory (DFT) calculations further confirm that the optimal electronic environment induced by Ni incorporation promotes the rearrangement of H–COO* intermediates and reduces energy barriers (Ebar), thus enhancing the catalytic activity. This work provides a cost-effective strategy for designing high-performance catalysts and promoting hydrogen storage technologies.
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高影响因子
Small
·
2025
·
IF 12.1
Qingmeng Guo,Fengting Li,Chongxi Zhang,Zhikun Wang,Zixi Kang,Lili Fan,Daofeng Sun
The strategic construction of heterostructures centered around Fe 2 P is proven to be effective for improving its performance in the oxygen reduction reaction (ORR) and zinc–air batteries (ZABs). In this study, SbZn is strategically employed to construct a novel Fe 2 P/SbZn heterostructure on N,P-doped carbon scaffolds, serving as an efficient electrocatalyst for the ORR in ZABs. Through a one-step pyrolysis of a Fe, Sb, P-incorporated zeolitic imidazolate framework, the Fe 2 P/SbZn@PNC catalyst is successfully synthesized. This catalyst demonstrates high ORR activity in alkaline media, achieving a half-wave potential of 0.936 V and a limiting current density of 6.18 mA cm −2 , both significantly surpassing those of commercial 20 wt% Pt/C. When applied in zinc–air batteries, the Fe 2 P/SbZn@PNC-based ZABs deliver a higher peak power density and superior long-term cycling stability compared to the Pt/C benchmark. Density functional theory (DFT) calculations reveal that the Fe 2 P/SbZn interface drives charge redistribution, optimizing the adsorption/desorption of oxygen intermediates and reducing the rate-determining energy barrier in ORR, thus enhancing catalytic activity. This innovative heterostructure provides new avenues for designing efficient electrocatalysts for energy conversion and storage.
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PubMed
高影响因子
ACS Omega
·
2025
·
IF 4.3
Chaofan Deng,Chun Cai
Pd–Cu bimetallic catalysts were successfully synthesized for the dehydrogenation of Bisphenol Z (BPZ) by an impregnation-reduction method. The obtained catalyst was studied by XRD, HRTEM, XPS, BET, and NH3-TPD techniques and effectively applied in the highly selective cleavage dehydrogenation of BPZ to give PPP > 99% yield at 270 °C and atmospheric pressure in the solvent-free condition. It was demonstrated that the “synergistic effect” of the bimetallic catalysts could effectively promote the cleavage dehydrogenation reaction. Pd species served as the primary active sites for the adsorption and dissociation of H* and the activation of C–H bonds, while the introduced Cu species accelerated the breaking process of the C–H bond. This catalyst demonstrated remarkable stability and could be reused over ten cycles without obvious decrease both in yield and selectivity. The likely reaction pathway was outlined to elucidate the cleavage dehydrogenation mechanism according to experimental results.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Xinyu Chen,Yingrui Nie,Wenqian Fan,Zhimin Zhao,Zhifei Wang,Yong Jiang
In this study, yolk-shell magnetic hydrogel microspheres loaded with silver nanoparticles (Fe 3 O 4 @P(DVB-co-MAA)@Ag) were innovatively constructed for efficient catalytic reduction of nitroaromatic compounds. First, hollow P(DVB-co-MAA) microspheres were prepared as shell. Fe 3 O 4 magnetic nanoparticles were successfully deposited into the microspheres as yolk through the decomposition of metal-organic precursor salts in high-temperature organic solvents. The EM images shows that Fe 3 O 4 @P(DVB-co-MAA) microspheres consist of a magnetic core, an intermediate void layer, and a hydrophilic hydrogel shell, demonstrating a unique multilayered structural feature. Then, highly active silver nanoparticles were uniformly loaded onto the hydrogel shell surface using the thermal co-reduction method. Catalytic results demonstrated that the yolk-shell material showed significantly enhanced activity toward the reduction of 4-nitrophenol (4-NP) and 2-nitroaniline (2-NA), compared to the core-shell structured composite microspheres. The catalytic parameters were 65.44 s⁻¹ g⁻¹ and 46.44 s⁻¹ g⁻¹ , respectively. Remarkably, the composite retained over 85 % catalytic efficiency after five cycles of use and achieved rapid magnetic separation within 20 s under an external magnetic field.
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RARE METALS
·
2024
·
IF 9.6
Liang Xin,Zhao Dong-Qing,Huang Qian-Qian,Liang Sheng,Wang Li-Li,Hu Lei,Liu Ling-Li,Hu Kun-Hong,Deng Chong-Hai,Cheng Sheng,Zhu Er-Tao,Deng Hua-Xia
Lithium–sulfur battery is one of the most promising battery systems for industrialization due to its high theoretical specific capacity and high energy density. Nonetheless, the “shuttle effect” has restrained the advancement of lithium–sulfur batteries. In this work, a gradient-structured nanofiber membrane with pure gelatin on one side and Super P-MoO 2 /MoS 2 -gelatin on the other side was created using a multi-step electrostatic spinning technique, which was applied for multi-functional separator for lithium–sulfur batteries. The pure gelatin layer facing the anode side primarily homogenizes the lithium flux, whereas the Super P-MoO 2 /MoS 2 -gelatin layer facing the cathode side primarily adsorbs polysulfides by physical and chemical adsorption and enhancing polysulfide conversion efficiency. The findings demonstrate that even after 150 cycles at 0.2C, the lithium–sulfur battery can still sustain a discharge-specific capacity of 572.3 mAh·g −1 . When used with Li||Li symmetric batteries, it has a cycle life of more than 1200 h. The commercialization of lithium–sulfur batteries is given a fresh idea by this straightforward preparation technique. Graphical abstract
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Zhouzhou Li,Zheng Li,Feng He,Wen He,Qixu Chen,Hongqing Wang
Recently, how to improve the photocatalytic uranium removal performance of Graphite-phase carbon nitride (GCN) has always been a hot research topic. In this paper, a new strategy based on p-n junction and D-A structure is proposed to improve the photocatalytic performance. And as a result, a novel cyano modified photocatalytic material NC-GCN/Ag 2 O was designed and prepared for the reduction of U(VI). Interestingly, the material shows better adsorption performance for U(VI) in the dark treatment stage, and its removal of U(VI) is close to 70 % under the initial U(VI) concentration of 20 ppm and the solid–liquid ratio of 0.2 g/L. And the adsorption is in accordance with the Langmuir model and Pseudo second order model. After 30 min of illumination, the removal rate of U(VI) can reach 93.2 %, significantly higher than that of GCN (13.6 %) and NC-GCN 10 (37.7 %). It’s worth mentioning that photocatalytic reduction dominated the adsorption-reduction process for U(VI) removal after light exposure. In addition, after four cycles, the removal of U(VI) from the composite material decreased by only 5 % with no change in the crystal structure, i.e., it has good reusability and stability. Meanwhile, there was no significant interference with other ions except for Cu 2+ and V 5+ , which had a weak interference. Finally, a new mechanism for U(Ⅵ) reduction was proposed.
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高影响因子
Advanced Energy Materials
·
2019
·Vol. 9
·期 12
·1802595
·
IF 24.884
Qin Zhou,Lusheng Liang,Junjie Hu,Bingbing Cao,Longkai Yang,Tingjun Wu,Xin Li,Bao Zhang,Peng Gao
Supported by the density functional theory (DFT) calculations, for the first time, a fluorinated aromatic cation, 2-(4-fluorophenyl)ethyl ammonium iodide (FPEAI), is introduced to grow in situ a low dimensional perovskite layer atop 3D perovskite film with excess PbI 2 . The resulted ( p -FC 6 H 4 C 2 H 4 NH 3 ) 2 [PbI 4 ] perovskite functions as a protective capping layer to protect the 3D perovskite from moisture. In the meantime, the thin layer facilitates charge transfer at the interfaces, thereby reducing the nonradiative recombination pathways. Laser scanning confocal microscopy unveils visually the distribution of the 2D perovskite layer on top of the 3D perovskite. When employing the 3D–2D perovskite as the absorbing layer in the photovoltaic cells, a high power conversion efficiency of 20.54% is realized. Superior device performance and moisture stability are observed with the modified perovskite over the whole stability test period.
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高影响因子
Materials
·
2025
·Vol. 18
·期 17
·4165
·
IF 3.2
Heng Zhang,Yiping Yang,Shengchao Yang,Yuchang Qin,Xuan Lv,Lin Cui,Wei Jia,Zhiyong Liu
The impact of encapsulating gemcitabine (GEM) into nanoparticles on its delivery remains underexplored, with the potential benefits of targeted drug delivery and stimuli-responsive release yet to be fully clarified. Herein, we designed a near-infrared (NIR) light-responsive polymeric nanoparticle, ZnPc@P(PEG-CMA-TKGEM), which integrates reactive oxygen species (ROS) generation and cell imaging capabilities. The self-assembled polymeric micelles exhibit a hydrodynamic size of ~134 nm. Under NIR irradiation, the cumulative drug release rate reaches 51% within 48 h, which is three times higher than that of the non-irradiated control group. In cytotoxicity assays, the cell viability of the NIR-irradiated drug-loaded group is approximately 17%, while that of the NIR-irradiated blank group (without drug loading) remains above 80%. These results confirm that the nanocarriers successfully deliver GEM to target cells and achieve controlled drug release via NIR stimulation.
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PubMed
高影响因子
CELLULOSE
·
2024
·Vol. 31
·期 6
·4007-4023
·
IF 4.9
Xue Tong,Ma Ruijie,Zhang Xintian,Tao Wenwen,Wang Chaoxia,Yin Yunjie
Personal thermal management (PTM) textiles with heating or cooling capabilities are highly attractive because they offer individual comfort and contribute to lower energy consumption. However, due to the subjectivity of thermal comfort, developing adaptive and personalized PTM textiles remains a challenge. Here, we report a thermoresponsive cotton fabric (PMOG-cotton), which is prepared by a combination of ultraviolet-induced free radical polymerization and pad-dry-cure process. 2-(2-methoxyethoxy)ethyl methacrylate (MEO 2 MA) and oligo(ethylene glycol) methacrylate (OEGMA 475 ) are selected as thermoresponsive monomers, while glycidyl methacrylate (GMA) is chosen as the linking monomer for copolymerization. The lower critical solution temperature (LCST) of P(MEO 2 MA-co-OEGMA 475 -co-GMA) can be precisely regulated by adjusting the dosage of OEGMA 475 . Furthermore, PMOG-cotton demonstrates a reversible transition between hydrophobic and hydrophilic states in response to variations in external temperature (T > LCST, hydrophobic; T < LCST, hydrophilic). This transition can be sustained for a minimum of 5 cycles and 50 rubbing cycles. PMOG-cotton exhibits superior control over breathability and moisture permeability compared to raw cotton in response to temperature fluctuations. Compared to raw cotton, PMOG-cotton offers a 2.4 °C heating effect in cold environments and a 1.3 °C cooling effect in hot environments. This adaptive thermal management textile shows promise for delivering human thermal comfort in complex and dynamic environments.
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高影响因子
PEST MANAGEMENT SCIENCE
·
2022
·Vol. 78
·期 6
·2240-2249
·
IF 4.462
Tan Dai,Zhiwen Wang,Xingkai Cheng,Huige Gao,Li Liang,Pengfei Liu,Xili Liu
BACKGROUND Fungicide resistance has become a serious problem for different mode of action groups except for uncouplers, which makes their resistance mechanism a hot topic, which until now, has not been well clarified. SYP-14288, a newly developed diarylamine fungicide modeled on fluazinam, has shown good toxicity to both oomycete and fungus by the action of uncoupling. In this research, the resistance of Phytophthora capsici to SYP-14288 was studied to clarify the resistance mechanism of uncouplers. RESULTS The toxicity tests of resistant strains against SYP-14288 showed multidrug resistance. The high-performance liquid chromatography (HPLC) results showed that resistant strains could efflux the fungicide, and this ability could be inhibited by the efflux pump inhibitor amitriptyline. The target protein of amitriptyline is P-glycoprotein (P-gp), which was overexpressed in resistant strains. Three products of nitrate reduction of SYP-14288 were detected and determined by HPLC-Q-TOF. Eight cytochrome P450 monooxygenase (P450) proteins were differentially involved in the reduction reaction. CONCLUSION Both fungicide efflux and detoxification metabolism were involved in the resistance mechanisms of P. capsici to SYP-14288. © 2022 Society of Chemical Industry.
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POLYMER DEGRADATION AND STABILITY
·
2020
·
IF 4.032
Wei Tao,Xu Hu,Jinhao Sun,Lijun Qian,Juan Li
Two phosphorus-nitrogen flame retardants were synthesized by using chlodiphenylphosphine (CDP) or diphenylphosphinyl chloride (DPP) and cytosine (Cy), respectively. The products are marked as CCDP and CDPP, and characterized by using Fourier transform infrared spectra (FT-IR), 31 P and 1 H nuclear magnetic resonance and thermogravimetric analysis (TGA). The CCDP and CDPP were used to modify the flame retardancy of polyamide 6 (PA6). The results indicated that 6 wt% CCDP and CDPP both make PA6 achieve the UL-94 V-0 rating and improve its LOI value. The degradation behavior was studied by TG-IR, melt volume-flow rate, etc. The results revealed that both CCDP and CDPP promote the degradation of PA6 and improve its flame retardancy by melting away. The CCDP tends to work in the gas phase and the CDPP in the condensed phase. In addition, in order to reduce the effect of flame retardant on the mechanical properties of PA6, CDPP was coated with epoxy resin . The results showed that the flame retardancy decrease after coating. Finally, melamine cyanurate was blended with the CDPP coated by epoxy to adjust the comprehensive properties of PA6 composite, and excellent flame retardancy and mechanical properties are obtained.
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高影响因子
Journal of Water Process Engineering
·
2020
·
IF 3.465
Xingyu Wu,Xingfu Song,Hang Chen,Jianguo Yu
Electrochemical oxidation process (EOP) has received attentions in wastewater management in recent years. However, high electrodes cost and low current efficiency have challenged the industrial application. Therefore, dimensional stable anodes (DSA) are developed due to relative low price and high efficiency of chlorinated active species generation. However, with low concentration of mediums, the direct oxidation still plays the main role in the organic pollutants degradation, resulting in low current efficiency of process. Thus, in this study, the impact of general operating conditions including type of electrolyte, active species addition, pH and current density on proportion of direct and indirect oxidation during p- nitrophenol degradation in DSA system have been studied, trying to enhance the contribution of indirect oxidation. The contribution was measured by scavenging tests. It concluded that low pH and adding NaClO can improve the contribution of indirect oxidation, but extra H 2 O 2 significantly hindered the PNP degradation. Furthermore, we have studied the behaviors of free radical reactions by quantum chemical calculation. Three mechanisms including hydrogen atom transfer (HAT), radical adduct formation (RAF) and electron transfer (ET) were discussed in hydroxyl free radical and chlorine-derived radicals reactions. According to calculated thermodynamic and kinetic parameters, it indicated that active sites in primary reactions initiated by OH are significantly more than that in chlorine-derived radical reactions, corresponding to the differences of experimental phenomenon under different mediums. Degradation pathways and main byproducts formation were also proposed. We provided an insight to study oxidation mechanisms of EOP by means of experiments combining quantum chemical calculation.
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高影响因子
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