CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yajie Feng,Chi Lin,Yifei Huang,Bing Li,Yingxin He,Jiangping Ma,Chaogang Ban,Lujie Ruan,Hongxing Jia,Xiaoping Tao,Liyong Gan,Xiaoyuan Zhou
The metal–metal interactions between different metal atoms within dual-metal-supported catalyst have garnered significant attention in effectively regulating the chemical and electronic structure of active sites, thus providing enormous opportunities to optimize the catalytic performance. Herein, by loading Cu clusters and Pd nanoparticles on TiO 2 (CuPd/TiO 2 ), it is found that Cu clusters enable the metalize transformation of Pd as a result of the metal–metal interactions between Cu and Pd, which remarkably improves the surface catalytic reaction as well as the separation and transfer of photogenerated carriers. The resultant photocatalyst exhibits an excellent activity for H 2 evolution coupled with benzyl alcohol oxidation, achieving yield rates of 43.7 μmol h −1 for H 2 and 22.0 μmol h −1 for benzaldehyde, and an apparent quantum efficiency (AQE) of 20.4 % at 313 nm for hydrogen evolution. This integration of metal–metal interactions within the dual-metal-supported catalyst open a new avenue for the design of advanced photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jun Zhang,Xinlan Xu,Lanyu Luo,Tiantian Peng,Boyu Liu,Lingying Jiang,Meng Jin,Rong Wang,Huan Yi,Weimin Wu,Shi-Yu Lu
The selective exposure of active surfaces has garnered exceptionally widespread attention in enhancing electrocatalytic performance for oxygen reduction reactions (ORR). Nevertheless, because unmanageable growth thermodynamics and kinetics, the exposure of active surface not only hinders the formation of high-index facets but also induces irreversible reconstruction of low-index facets at high-potential region. Therefore, the controlled synthesis of Pd-based nanocrystals featuring high/low-index facets is highly desirable. In this study, bimetallic PdNi alloys with high/low-index facets were successfully synthesized through crystal structure engineering. Assisted by Ni 2+ , the transition from low-index facets to high-index facets was achieved. These structural features endow PdNi alloy nanocrystals with highest half-wave potential (0.893 V), mass activity (0.127 A mg −1 ), and specific activity (0.926 mA cm −2 ) in ORR. Additionally, this alloy nanocrystals follow an efficient four-electron reduction pathway and exhibit excellent long-term stability over 10,000 cycles. Density functional theory calculations suggest that the outstanding ORR performance stems from the minimal downhill energy gradient in the rate-determining step, and the reduced oxygen adsorption energy on the PdNi alloy (311) crystal plane. This innovative strategy adds more potentialities for development and commercial application in fuel cells.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Wen-Wang Yu,Xiang-Guang Meng,Wen Li,Li-Yu Chen,Zi-Yu Gan,Yu-Lian Zhang,Jie Zhou
Chemical conversion of CO 2 to cyclic carbonates is one of the most attractive strategies for CO 2 capture and storage utilization. Herein, a binary organocatalyst of 3-aminobenzylalcohol/ n -Bu 4 NI was used to gently catalyze the insertion of CO 2 into the terminal/internal epoxides to generate cyclic carbonates under metal-free and solvent-free conditions. Twelve representative terminal epoxides reacted with CO 2 to achieve excellent cyclic carbonate yields of up to 98.3 % at 30 °C and 1 atm CO 2 and six low activity internal di-substituted epoxides were converted to corresponding cyclic carbonates with yields of up to 96.2 %. Experiments on actual flue gas and water resistance revealed the potential industrial value of this binary organocatalyst. The yield of cyclic carbonate reached 99 % by using actual flue gas under very mild conditions of 60 °C and 1 atm. The results of 4-fold epoxide amplification experiment showed that the residual CO 2 in the flue gas was only 793 ppm after reaction at 1 atm and 60 °C, indicating the good CO 2 capture and conversion ability. Reaction kinetics and catalytic mechanism of the cycloaddition were investigated in detail. The synergistic effect among functional groups of catalysts on substrates is the essential factor for the high activity of the catalyst.
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EUROPEAN POLYMER JOURNAL
·
2024
·
IF 5.8
Hongwei Wang,Yaoping Lu,Hehang Sun,Chunping Hou,Bolin Gong,Junjie Ou
With an increasing requirement for functional materials, anisotropic Janus particles have gradually developed into highly attractive materials in catalysis, drug delivery, lotion stabilizer and other fields. Herein, non-crosslinked poly(glycidyl methacrylate) (poly(GMA)) served as seed particle, GMA and trimethylolpropane trimethylacrylate (TMPTMA) were utilized as functional monomer and crosslinker, respectively. The composition of water phase consisted of polyvinyl alcohol (PVA) and sodium dodecyl sulfonate (SDS), and 2,2-dimethoxy-2-phenylacetophenone served as photo-initiator. A series of Janus particles with asymmetric morphologies such as lychee-like, acorn-like, half raspberry-like and hamburger-like were fabricated via seed-swelling photoinitiated polymerization. In addition, several parameters such as the ratio of monomers and crosslinker and the type of porogenic solvent were adjusted to improve the anisotropy, dispersity and uniformity. Subsequently, Janus carbonaceous particle was acquired via calcination and utilized as an anode material for lithium-ion batteries. The relevant properties were measured via electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), cyclic performance and constant current charging and discharging testing, demonstrating better performance for electrochemistry. After the second cycle, the stable coulombic efficiency of 95.24% over 100 cycles. Thus, our strategy provides an excellent insight for fabricating Janus carbonaceous particle with controllable morphology, and is expected to have applications in other fields.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yunfei Sun,Yaping Wang,Yun Chen,Junchao Qian,Feng Chen,Zelong Zhou,Chaoya Han,Yu Shi,Xiaowang Lu,Chaoying Ni
Bisphenol A (BPA), a prevalent organic pollutant found in wastewater environment, is notorious for its resistance to natural degradation, raising significant ecological and human health concerns. In this study, a “signal-on” photoelectrochemical aptasensing system was designed for detecting BPA in real water samples with high specificity and sensitivity. One-dimensional (1D) β-FeOOH nanobelts were synthesized on a two-dimensional (2D) porous carbon nitride (g-C 3 N 4 ) through an in-situ growth procedure. The β-FeOOH/g-C 3 N 4 nanocomposites demonstrated superior photoelectric conversion efficiency due to several factors: (i) The 1D nanobelt-like structure of β-FeOOH shortens the charge transfer path within the nanocomposite, enabling directional and rapid migration of photoinduced charges from the interior to the surface. (ii) β-FeOOH possesses strong visible absorption capabilities, enhancing the utilization of g-C 3 N 4 under photoexcitation, resulting in the generation of numerous photo-induced carriers. (iii) The in-situ formation of the β-FeOOH/g-C 3 N 4 heterojunction establishes an intimate interfacial contact, facilitating the rapid separation and transfer of charges between β-FeOOH and g-C 3 N 4 . A photoelectrochemical aptasensing platform based on the photoactive material of β-FeOOH/g-C 3 N 4 detects BPA with reduced photocurrent owing to the presence of BPA-aptamer macromolecules on the electrode surface. This BPA detection system exhibits excellent linearity over a wide concentration range from 10 pM to 10 nM, with high sensitivity (a detection limit of 3.5 pM), stability, specificity, and repeatability. Furthermore, this research offers a straightforward and rapid sensing platform for monitoring BPA enriched water environments.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Cai Xu,Shandi Zhong,Lei Yuan,Mincheng Yu,Yingqi Chen,Liyan Dai,Xiaozhong Wang
It is desired but challenging to develop a non-noble metal catalyst for the selective oxidation of benzyl alcohol with O 2 under solvent-free conditions. Herein, a series of Ce-doped high entropy oxides (Ce/HEOs) were prepared via co-precipitation and subsequent thermal treatment method. It was found that, the doping of Ce could remarkably promote the catalytic activity for selective oxidation of benzyl alcohol to benzaldehyde. The improved activity was ascribed to the good distribution of active Ce species, the increased oxygen vacancies, and the synergistic effect between CeO 2 and high entropy oxides (HEOs). In addition, the surface oxygen of Ce/HEOs towards Ce displayed stronger reducibility compared to that of bare CeO 2 , endowing it stronger deprotonation ability towards benzyl alcohol during the reaction. The prepared catalyst exhibited satisfactory reusability and stability owing to the entropy-stabilized effect of HEOs and the interaction between CeO 2 and HEOs, and negligible loss in catalytic activity was observed after seven runs. Besides, DFT calculations disclosed that, with the doping of Ce, the Ce/HEOs catalyst possessed stronger adsorption ability towards benzyl alcohol, and lower free energy was required for the rate-determining step during the whole oxidative reaction. This work gave some insights into the promotional effect of Ce doped into high entropy oxides for the solvent-free catalytic oxidation of benzyl alcohol.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 2
·1-12
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IF 5.3
Xu Ning,Li Xin,Tian Chunyuan,Zhang Zhiyang,Chen Lingxin,Luan Feng,Zhuang Xuming
A lanthanide ion–based metal–organic framework (Eu-TATAB nanorods) was designed and synthesized as an effective tri-mode nanoprobe for sensitive and portable detection of ethanol content in a water–ethanol mixture. The assay was based on the responsive properties of Eu-TATAB nanorods to ethanol stimulus and their adaptive encapsulation capability towards optically active lanthanides. With the addition of ethanol to the Eu-TATAB nanorods, the structure was destroyed, resulting in a decrease in luminescence, electrochemiluminescence, and ultraviolet–visible spectrophotometric signals by perturbing energy transfer in the Eu-TATAB nanorods. According to the degree of the decrease in three luminescence intensities, the ethanol content could be quantitatively detected. Based on this, the rapid detection of alcohol content in different types of spirits and alcoholic beverages was further realized. This method is simple, convenient, and sensitive, and has good application prospects and development potential. Graphical
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Liyi Tang,Yangsen Xu,Shuang Tang,Yu-Xiang Yu,Aiyun Meng,Xinzhong Wang,Wei-De Zhang
Photocatalytic hydrogen production utilizing solar energy provides a pivotal strategy for realizing a carbon–neutral society. Cocatalyst-modified semiconductor materials have emerged as promising candidates for photocatalytic applications due to their ability to facilitate the spatial separation and directional migration of photogenerated electron-hole pairs. Nevertheless, those systems often face challenges such as intricate preparation procedures and issues with non-compact recombination. Herein, we report a one-pot thermal treatment approach for synthesizing a composite of Mn 3 O 4 nanoparticles and sodium poly(heptazine imides) (Na-PHI). Mn 3 O 4 nanoparticles were in situ generated and embedded within the Na-PHI matrix during the sintering process. The resulted photocatalyst demonstrated significantly enhanced photoinduced charge separation efficiency, exhibiting approximately 6-fold and 3-fold improvements compared to pristine Mn 3 O 4 and Na-PHI, respectively. The photocatalytic hydrogen evolution rate reached 14 μmol h −1 , nearly 14 times that of Na-PHI (1.2 μmol h −1 ) in the aqueous solution of benzylamine (BA) under visible light illumination (780 nm ≥ λ ≥ 420 nm). Furthermore, the optimized Mn 3 O 4 -Na-PHI sample (Mn-Na-PHI) displayed a remarkably high photocatalytic hydrogen generation rate alongside the synchronous photo-oxidative coupling of aliphatic and aromatic amine under visible light. This work underscores the potential for rational design and synthesis of novel Na-PHI-based functional composites for sustainable energy applications.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 24
·10820-10829
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IF 2.7
Weichuan Xu,Hong Huang,Lingling Bi,Haimei Xu,Zhichao Miao,Mei Wu
Carbonyl compounds serve as essential raw materials in the production of fine chemicals and pharmaceuticals. An economical and environmentally-friendly route to generating carbonyl compounds involves the catalytic oxidation of alcohols and hydrocarbons using heterogeneous catalysts. In this work, we synthesize a series of vanadium-doped ordered mesoporous zirconium oxophosphate (V/M-ZrPO) nanocomposites via a modified one-pot evaporation-induced self-assembly approach. Characterization results confirm the successful embedding of vanadium species into the framework of the M-ZrPO support. Dispersion of vanadium sites generates catalysts exhibiting enhanced performance for the selective oxidation of alcohols and hydrocarbons to carbonyl compounds. In particular, the 20 V/M-ZrPO catalyst demonstrates excellent reusability and broad substrate compatibility. Relative to established catalytic materials, the 20 V/M-ZrPO catalyst demonstrated superior performance across key metrics including product yield, reaction time, and recyclability. These findings highlight the promise of V/M-ZrPO nanocomposites as efficient and durable catalysts for sustainable carbonyl compound production.
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Nanomaterials
·
2024
·Vol. 14
·期 9
·744
·
IF 4.4
Xin Pan,Yanan Zhu,Yongchang Yang,Qianqian Zhu
The catalytic oxidation of alcohols is an important transformation in the chemical industry. Carbon materials with a large surface area and N doping show great promise as metal-free catalysts for the reaction. In this study, a rich N-containing covalent triazine framework polymerized by cyanuric chloride and p-phenylenediamine was used to synthesize N-doped porous carbon with the assistance of a pore-forming agent—NaCl. First, the mass ratio of the polymer/NaCl was optimized to 1:9. Then, the influence of the pyrolysis temperatures (700–1000 °C) on the materials was studied in detail. It was found that the carbon materials were gradually exfoliated by molten salt at high temperatures. XRD and Raman characterizations showed them with a certain graphitization. The optimal doped carbon CNN-1-9-900 achieved the highest surface area of 199.03 m2g−1with the largest pore volume of 0.29 cm3g−1. Furthermore, it had a high N content of 9.9 at% with the highest relative proportion of pyridinic/graphitic N. Due to the synergistic effect between the surface area and pyridinic/graphitic N, CNN-1-9-900 showed the best performance for benzyl alcohol oxidation with TBHP at moderate conditions, and the process also worked for its derivatives.
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Nanomaterials
·
2024
·Vol. 14
·期 14
·1188
·
IF 4.4
Hongyang Wu,Chen Chen
The efficient detection of n-butanol, which is in demand for highly sensitive materials, is essential for multiple applications. A nonaqueous method was applied to prepare NiFe2O4nanoparticles (NPs) using benzyl alcohol as a solvent, which shows a size of 7.9 ± 1.6 nm and a large surface area of 82.23 m2/g. To further improve the sensing performance for n-butanol, Pd/PdO functionalization was sensitized with NiFe2O4NPs. Gas sensing results demonstrate that the Pd/PdO-NiFe2O4exhibits an enhanced response of 36.9 to 300 ppm n-butanol and a fast response and recovery time (18.2/17.6 s) at 260 °C. Furthermore, the Pd/PdO-NiFe2O4-based sensor possesses a good linear relationship between responses and the n-butanol concentration from 1 to 1000 ppm, and great selectivity against other volatile organic compounds (VOCs). The excellent sensing enhancement is attributed to the catalytic effects of Pd/PdO, the increase of oxygen vacancies, and the formation of heterojunction between PdO and NiFe2O4. Thus, this study offers an effective route for the synthesis of Pd/PdO-functionalized NiFe2O4NPs to achieve n-butanol detection with excellent sensing performance.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Dandan Song,Guoqiang Li,Qian Liu,Xingge Huang,Weiyu Wang,Faming Gao
The accurate monitoring of pesticide residues in agricultural products is critical for maintaining food quality and human health. The development of innovative analysis techniques capable of satisfying the stringent demands of practical applications is the key to building intelligent and highly-efficient pesticide detection equipment. Here, an ultrasensitive electrochemical biosensor has been reported, which utilizes quinary PtPdRhFeCu high-entropy alloy mesoporous nanotubes (PtPdRhFeCu HEA mNTs) and N/Cu dual-atom anchored ZnSe@C (N-Cu-ZnSe@C) as electrode materials. Multi-effect coupling (defect effect, high entropy effect, lattice distortion effect and doping effect), endows the proposed sensing interface with extremely high electronic conductive properties and unprecedentedly large electroactive surface area, which could heavily promote the charge transfer capability, meanwhile assists the acetylcholinesterase (AChE) with high affinity towards its substrate, thereby significantly improving the pesticide analysis performance of the sensor. Remarkably, the detection limit of this assembled biosensor for aldicarb sulfone and methamidophos detection are notably low at 2.32 fM and 4.58 fM, respectively. Moreover, this biosensor demonstrated wide detection ranges (7 pM ∼ 70 nM for methamidophos and 1 pM ∼ 0.1 μM for aldicarb sulfone), high sensitivity and specificity, along with good recovery rates (86.67 % ∼ 117.14 %) in real samples. This signal amplification strategy enhances the analysis capability by integrating multiple effects, and provides an innovative analysis tool for hazardous substance analysis in food safety and environmental monitoring research.
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