Nature Communications
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2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Long Haoyu,Zhang Xidong,Zhang Zhenyi,Zhang Jianjun,Yu Jiaguo,Yu Huogen
The H 2 -evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H ads /H des ) still remains a great challenge. Herein, we propose a fine-tuning d - p hybridization strategy to precisely optimize the H ads /H des kinetics in a Ni-B x modified CdS photocatalyst (Ni-B x /CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B x cocatalyst gradually strengthens the d - p orbital interaction between Ni 3 d and B 2 p , resulting in a consecutive d -band broadening and controllable d -band center on Ni active sites. The above consecutive d -band optimization allows for precise modulation of the H ads /H des dynamics in the Ni-B x /CdS, ultimately demonstrating a remarkable H 2 -evolution activity of 13.4 mmol g -1 h -1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B x /CdS photocatalyst. This work provides insights into the optimal design of prospective H 2 -evolution catalysts.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Shu Li,Xinyu Chen,Qingzhen Tian,Jinjin Liu,Zheng Tang,Xiangheng Niu
Organophosphorus pesticides (OPs) are widely used in agricultural production, posing a great threat to human health and the environment. Given that different OPs present different toxicology and toxicities, identifying individual pesticide residues becomes important for assessing food safety and environmental implications. In this work, a kinetics difference-driven analyte hydrolysis strategy is proposed for the first time and validated to identify p-nitrophenyl pesticides by developing an organophosphorus hydrolase-like nanozyme-coded sensor array. Ultrasmall bare CeO2 nanoparticles were synthesized and employed as the only sensing unit to catalyze the hydrolysis of multiple analytes. With catalytic preferences and kinetics differences under identical reaction conditions, five common OPs analogues (methyl-paraoxon, paraoxon, methyl-parathion, parathion, and fenitrothion) offered discriminable colors. By coupling the color fingerprints with pattern recognition, the accurate identification of individual p-nitrophenyl pesticides and their mixtures at a variety of concentrations and ratios was verified in laboratory and practical scenarios. Attractively, apart from excellent performance and convenient operation, the proposed hydrolytic nanozyme-coded pattern presents strong resistance against redox substances that often cause interference in previous oxidoreductase-based sensor arrays. Our study provides a new paradigm of discriminating specific OPs precisely, showing promising applications in multitarget analysis in complex matrices.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Chenglong Ding,Yao Li,Wenfei Xiao,Qi Chen,Yanming Li,Jingfu He,Changli Li
Constructing p-Si based heterojunction photocathode is a promising means to convert solar energy into storable hydrogen fuel . The favorable energy band alignment between p-Si absorber and electron transport layer (ETL) is crucial to realize efficient photogenerated carrier separation and transport during photoelectrochemical water splitting . The trade-off between large Fermi level difference and optimized conduction band offset (CBO) in p-Si heterojunction is a major limiting factor for achieving high solar-to-hydrogen efficiency. Herein, we introduced a double CdS/In 2 S 3 ETLs on p-Si to optimize band alignment and facilitate the charge carrier transport at the interface. The p-Si/CdS/In 2 S 3 system presents a step-like energy band alignment and the appropriate CBO at p-Si/CdS (0.46 eV) and CdS/In 2 S 3 (0.25 eV) interface suppress the charge recombination and efficiently extract photogenerated electrons. The Electrochemical impedance spectroscopy measurement shows a lower charge transfer resistance for the double ETLs compared with the single ETL counterparts. As a result, the p-Si/CdS/In 2 S 3 /Pt photoelectrode exhibits a positive onset potential of ∼0.5 V RHE and a high applied bias photo-to-current efficiency of 5.6 % under AM 1.5G illumination. The strategy of band alignment engineering provides an effective way to improve the device performance and can be extended to other emerging semiconductor thin film photocathodes.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Qingtian Xu,Jierui Ye,Shuaibo Han,Yuebing Gao,Pan Chen,Siqun Wang,Qiang Wu,Qian Li
Renewable polymeric microcapsules hold promise for precisely controlled release of hydrophobic drugs (curcumin) in therapeutic treatment. However, there still remains challenges to stabilize the properties of microcapsules and to enhance encapsulation efficiencies of curcumin. By using an eco-friendly ternary deep eutectic solvent here, we successfully fabricated native cellulose nanofibrils, holocellulose nanofibrils, and lignocellulose nanofibrils containing both phytates and sulfate groups. In addition, a novel type of curcumin-loaded polymeric microcapsules with diameter of 10–20 μm were prepared by cellulose nanofibrils as stabilizing agents in Polylactide Pickering emulsion. The Pickering emulsions stabilized by P/N/S-containing cellulose nanofibrils, holocellulose nanofibrils, and lignocellulose nanofibrils are more stable than the unmodified cellulose nanofibrils-stabilized emulsion. The Pickering emulsion stabilized by 0.2 wt% P/N/S-containing lignocellulose nanofibrils exhibited the highest emulsion layer height and the zeta potential reached −39.74 ± 2.88 mV. Moreover, the highest encapsulation efficiency of curcumin can be up to 94.80%. Antimicrobial test revealed that curcumin in the polymeric microcapsules exhibited an excellent inhibitory effect on S. aureus and the antibacterial efficiency reached 98.66%. These results provided important information on the comparison of different cellulose nanofibrils-stabilized Pickering emulsions and the application of controlled release of curcumin incorporated polymeric microcapsules in drug delivery system.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2018
·Vol. 96
·期 11
·2443-2449
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IF 1.265
Jiaming Xue,Zuoxiang Zeng,Weilan Xue,Huayu Yang
The kinetics of the esterification between benzoic acid and isoamyl alcohol has been studied using p -toluenesulphonic acid as a catalyst. The conversion of the benzoic acid was determined by following the concentration of water measured with a Karl Fischer titrator. The effects of the reaction temperature, catalyst concentration, and initial acid to alcohol molar ratio on reaction kinetics have been examined. A five-step assumption was proposed to describe the reaction mechanism for the formation of isoamyl benzoate. And the kinetic model derived from the proposed mechanism can fit well with experimental kinetic data of the esterification, which indicates that the proposed mechanism is reasonable. The nonideality of the liquid reaction mixture has been considered and the activity coefficients of all components were estimated by the UNIFAC model. The reaction rate constants from 353.15 K to 383.15 K have been determined through the least square method. Meanwhile the activation energy and the standard enthalpy change of reaction in the presence of p -toluenesulphonic acid were calculated to be 50.45 kJ/mol and −3.75 kJ/mol respectively.
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Nanoscale
·
2018
·Vol. 10
·期 13
·6186-6193
·
IF 7.233
Meiling Chen,Yufeng Wu,Weixing Song,Yuncheng Mo,Xiankun Lin,Qiang He,Bin Guo
High-performance floating film-based solar steam generation has received extensive attention for clean fresh water generation. Herein, we report high-strength nanoporous gold nanoparticle (AuNP)/poly(p-phenylene benzobisoxazole) nanofibre (PBONF) composite films that are capable of enhanced solar steam generation. The PBONFs were employed as building blocks to fabricate nanoporous PBONF multilayer composite films using a layer-by-layer assembly technique. These PBONF multilayer composite films then served as supports for depositing AuNPs. The resulting AuNP/PBONF composite films exhibit a high strength of 122 MPa and Young's modulus of 3.7 GPa, a broad spectrum photothermal effect, a mesoscopic structure, and a low thermal conductivity of 0.230 W m−1 K−1. Under one sun exposure, the AuNP/PBONF composite films exhibit an evaporation rate of 1.424 kg m−2 h−1 and a solar-vapor conversion efficiency of 83%. The AuNP/PBONF composite films are stable; therefore, they can be readily reused. These high-performance AuNP/PBONF composite films have potential for clean water generation under some extreme conditions such as space environments.
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Energy Technology
·
2025
·
IF 3.6
Yueqin Zhao,Yuxin Sun,Liuyun Chen,Xianjun Yang,Pengfei Yang,Xinling Xie,Zuzeng Qin,Hongbing Ji,Tongming Su
Photocatalytic hydrogen production from water splitting is a promising technology for overcoming energy and environmental issues. Herein, Mn 0.4 Cd 0.6 S/CuS composites were constructed for photocatalytic hydrogen production. The amount of CuS is optimized, and the composition and structure of the Mn 0.4 Cd 0.6 S/CuS composite are investigated via various characterization techniques. The formation of a p–n heterojunction between Mn 0.4 Cd 0.6 S and CuS and the built-in electric field improve the separation efficiency of photogenerated electrons and holes and enhance the performance of photocatalytic hydrogen production. When the content of CuS is 5 wt%, Mn 0.4 Cd 0.6 S/5CuS presents the best photocatalytic hydrogen production rate of 22.10 mmol h −1 g −1 , which is 3.0 times greater than that of Mn 0.4 Cd 0.6 S, and the apparent quantum yield reaches 7.82% at 400 nm. Combined with the activity test and characterization results, the reaction mechanism of photocatalytic hydrogen production over the Mn 0.4 Cd 0.6 S/CuS composite is proposed.
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GREEN CHEMISTRY
·
2024
·Vol. 27
·期 1
·133-143
·
IF 9.3
Hongjiao Chen,Kewei Zhang,Yanzhi Xia,Jian Li,Bin Hui
Coupling the urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) in seawater is desirable to produce sustainable and green hydrogen due to the reduced energy consumption. However, developing high-performance UOR/HER electrocatalysts in seawater instead of pure water remains a great challenge. Herein, (B,P,Co,Fe)-Ni anchored on Paulownia Wood (PW) is proposed to enhance the overall urea-(sea)water splitting performance. The resulting sample only needs a potential of 1.34 V to deliver a large current density of 100 mA cm−2 for alkaline UOR and features a remarkable durability to maintain 100 mA cm−2 for 100 h. The HER and UOR (HER||UOR) coupled system in alkaline seawater-urea electrolyte for producing H2 demonstrated a more significantly reduced electrolyzer voltage of 1.67 V obtained at 100 mA cm−2 in comparison to that of the HER||OER system (1.98 V). The well-aligned micro-channels and nanopores in wood frameworks not only improve the hydrophilicity and aerophobicity of the whole electrode, which is conducive to the penetration of the electrolyte and release of bubbles, but also shorten the transmission distance of ions and intermediates to accelerate the reaction kinetic process. Density functional theory calculations reveal that Co, Fe, P and B co-doping in Ni effectively adjusts the electronic structure, and the adsorption/desorption behavior of the urea reaction intermediates is regulated by the synergistic effect from multiple components, resulting in an excellent catalytic activity in seawater-urea media. This work promotes a better understanding of the surface electronic structure modulation of nanowood via doping strategy and offers great potential in the design of advanced UOR/HER catalysts for hydrogen production and urea wastewater treatment.
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JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Shengzu Xiao,Zhengyao Sun,Zehao Zhang,Pin Ma,Haibo Li
The application of Mo 2 CT x MXene as an anode for lithium-ion batteries (LIBs) is severely limited by the little electrochemical active sites and large diffusion energy barrier of lithium ions. Creating heterostructures between MXene and high-performance secondary materials with unique structure and tunable electron arrangement is an effective strategy. Herein, the heterostructure of P-doped MoO 2 and Mo 2 CT x (Mo 2 CT x /MoO 2 -P) with built-in-electric field and rich oxygen vacancies is constructed to co-regulate the electrochemical performance of battery. This design enables the material with high electronic density of states, improved ability of lithium adsorption and diffusion as well as strong structural stability. As a result, the as-prepared Mo 2 CT x /MoO 2 -P anode delivers excellent rate performance (301.3 mAh g −1 at 5 A g −1 ) and long cycle stability (1062.13 mAh g −1 at 1350 cycles at 2 A g −1 and 345.5 mAh g −1 at 4500 cycles at 5 A g −1 ), which are superior to that of previously reported Mo 2 CT x -based anode materials. Moreover, the Mo 2 CT x /MoO 2 -P||LiCoO 2 full cell offers 341.4 mAh g −1 after 200 cycles at 1 A g −1 , confirming the practicality of Mo 2 CT x /MoO 2 -P.
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POLYMERS FOR ADVANCED TECHNOLOGIES
·
2011
·Vol. 23
·期 10
·1329-1334
·
IF 1.776
Nianjun Kang,Zhongjie Du,Hangquan Li,Chen Zhang
In this report, a novel phosphorus/silicon-containing reactive flame retardant, hexa(3-triglycidyloxysilylpropyl)triphosphazene (HGPP), was synthesized and characterized by Fourier transform infrared spectrometry and nuclear magnetic resonance spectra ( 1 H, 31 P, and 29 Si), respectively. To prepare cured epoxy, HGPP had been co-cured with diglycidyl ether of bisphenol-A (DGEBA) via 4,4-diaminodiphenylsulfone as a curing agent. The mechanical, thermal, and flame retardant properties of the cured epoxy were evaluated by dynamic mechanical analysis, thermogravimetric analysis, and limiting oxygen index (LOI). According to these results, it could be found that incorporation of HGPP in the cured epoxy system showed good thermal stability, high LOI values, and high char yield at high temperature. As moderate loading of HGPP in the epoxy system, its storage modulus and glass transition temperature were higher than those of neat DGEBA. Copyright © 2011 John Wiley & Sons, Ltd.
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Materials
·
2024
·Vol. 17
·期 13
·3046
·
IF 3.1
Xiang Ke,Lifang Deng,Yanping Wang,Kai Tang,Lei Xiao,Gazi Hao,Peili Li,Xiang Zhou
Strengthening the interfacial contact between the reactive components effectively boosts the energy release of energetic materials. In this study, we aimed to create a close-knit interfacial contact condition between aluminum nanoparticles (Al NPs) and Polyvinylidene fluoride-hexafluoropropylene (P(VDF-HFP)) through hydrolytic adsorption and assembling 1H, 1H, 2H, 2H-Perfluorododecyltrichlorosilane (FTCS) on the surface of Al NPs. Leveraging hydrogen bonding between –CF and –CH and the interaction between C–F⋯F–C groups, the adsorbed FTCS directly leads to the growth of the P(VDF-HFP) coating layer around the treated Al NPs, yielding Al@FTCS/P(VDF-HFP) energetic composites. In comparison with the ultrasonically processed Al/P(VDF-HFP) mixture, thermal analysis reveals that Al@FTCS/P(VDF-HFP) exhibits a 57 °C lower reaction onset temperature and a 1646 J/g increase in heat release. Associated combustion tests demonstrate a 52% shorter ignition delay, 62% shorter combustion time, and a 288% faster pressurization rate. These improvements in energetic characteristics stem from the reactivity activation of FTCS towards Al NPs by the etching effect to the surface Al2O3. Moreover, enhanced interfacial contact facilitated by the FTCS-directed growth of P(VDF-HFP) around Al NPs further accelerates the whole reaction process.
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JOURNAL OF FLUORESCENCE
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2024
·
IF 2.6
Dai Zhengyuan,Liu Hao,Sun Xuyuan,Wang Ying,Fan Jie,Li Li,Ding Yaping
Using o-phenylenediamine as carbon source and phytic acid as phosphorus source, two P-rich carbon quantum dots RCDs and BCDs were synthesized successfully by changing the reaction temperature and time of hydrothermal method. It was found that RCDs with red emission could realize sensitive detection of 2-methylimidazole, and 2-methylimidazole had no obvious quenching effect on BCDs with blue emission, which made RCDs a sensitive, quick and selective fluorescence sensor for 2-methylimidazole detection. Under the optimal experimental conditions, the fluorescence intensity of RCDs decreased with the increasing of 2-methylimidazole concentration. The detection of 2-methylimidazole concentration by the carbon quantum dots sensor showed a good linear relationship in the range of 5 ~ 110 µM, and the low detection limit was 0.61 µM (S/N = 3). The sensor is able to detect 2-methylimidazole in lake water, enabling the application of real samples. The results show that this work provides a simple fluorescence method to detect 2-methylimidazole in water.
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