CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Chaochen Wang,Wangxin Ge,Lei Tang,Yanbin Qi,Lei Dong,Hongliang Jiang,Jianhua Shen,Yihua Zhu,Chunzhong Li
ABSTRACT Metal single-atom/atomic cluster catalysts (SA/AC) have emerged as effective electrocatalysts for the CO 2 reduction reaction (CO 2 RR) due to their high metal atom utilization and controllable metal coordination environments. However, the designing and tuning of the local electronic environments of SA/AC ensembles remain a significant challenge. In this work, we develop a single-atom-modified atomic cluster copper catalyst (Cu SA/ACs) for CO 2 RR. The SA/AC-induced modulation of the local electronic structure enhances CO 2 adsorption on the atomic cluster; additionally, the atomic cluster provides abundant active hydrogen for CO 2 protonation by mediating hydrolysis dissociation on the SAs. Consequently, compared to copper single-atom catalysts (Cu SACs), the Cu SA/ACs exhibit significantly improved activity, the current is 3.6 times that of Cu SACs, and the Faradaic efficiency of CO rose from 27.15% to 98.94%. The Cu SA/ACs catalyst can efficiently reduce CO 2 to CO in flow-cell configuration, and the CO selectivity is 93.06% at a current density of 600 mA cm –2 . The maximum energy efficiency of the cathode is 61.9%, which is superior to that of most CO 2 -to-CO catalysts. This work provides a new perspective for developing efficient SA/AC catalysts.
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ACS Applied Polymer Materials
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2024
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IF 4.4
Jiayi Gan,Jie Zhou,Yusong Xu,Tao Zhang,Xianming Zhang
Waterborne polyurethane (WPU) has promising application prospects in paints and coatings owing to its low volatile organic compounds (VOCs), excellent abrasion resistance, and mechanical properties. However, WPU is highly flammable, and there is a high demand for its antibacterial properties in practical applications. To date, effectively suppressing melt dripping remains a challenge during combustion and imparts a high antibacterial property to WPU without compromising the inherent mechanical property. Herein, we report WPU composites on the basis of a Cu(II)–phytate–aromatic Schiff base complex prepared from an aromatic Schiff base derivative, copper(II) acetate, and green and renewable phytic acid. The resultant WPU composites achieved a limiting oxygen index (LOI) of 27.5%. In the UL-94 test, they achieve a UL-94 V-0 rating with no molten droplets and self-extinguish within 1 s after the first and second flame applications. Meanwhile, smoke emission is effectively inhibited in the cone calorimetry test. Moreover, the WPU composites exhibit a killing rate of 99.9% against Staphylococcus aureus and Escherichia coli and excellent tensile toughness, providing a useful reference for designing and fabricating flame-retardant and antibacterial WPU composites.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qiujiang Li,Xuanyu Xiao,Tianyou Yan,Dan Song,Lei Li,Zhiyu Chen,Yuting Zhong,Wei Deng,Xiaoyan Liu,Yueming Song,Lei Wang,Yunbing Wang
The complex microenvironment of persistent inflammation and bacterial infection is a major challenge in chronic diabetic wounds. The development of nanozymes capable of efficiently scavenging reactive oxygen species (ROS) is a promising method to promote diabetic wound healing. However, many nanozymes show rather limited antioxidant activity and ROS-dependent antibacterial effects under certain circumstances, further weakening their ability to scavenge ROS. To meet these challenges, electronically regulated bioheterojunction (E-bio-HJ) nanozyme hydrogels derived from metal–organic frameworks (MOFs) were designed and prepared via an interface engineering strategy. Owing to the electron transfer and redistribution effects of the abundant and highly dispersed Cu–O–Zn sites at the heterogeneous interface, the E-bio-HJ nanozymes exhibited catalase (CAT)-like activity with ultrahigh hydrogen peroxide affinity (Km = 25.76 mM) and sustained ROS consumption. In addition, owing to the enhanced interfacial effect of E-bio-HJ and the good biocompatibility and cell adhesion of the methacryloylated gelatin (Gel) hydrogel, the E-bio-HJ gelatin hydrogel (E-bio-HJ/Gel) further reduced inflammation by inducing macrophage transformation to the M2 phenotype, accompanied by excellent antimicrobial properties and enhanced cell migration, angiogenesis, and collagen deposition, which synergistically promoted diabetic wound healing. This highly effective and comprehensive strategy offers a new approach for the rapid healing of diabetic wounds.
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JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Jianxian Li,Wenting Lin,Minglei Lu,Junwei Liao,Changsong Hu,Tiejun Wang
Efficient release of H 2 with negligible CO impurities from sustainable MeOH/H 2 O has become a promising goal for on-board hydrogen generator. However, hydrogen release kinetics still face challenges. In this work, the Cu/ZnO/CeO 2 catalyst with high density ultra-small Cu nanoparticles and abundant oxygen vacancies were prepared for intensifying hydrogen evolution in aqueous phase reforming of methanol (APRM). The optimized 55% Cu/ZnO/CeO 2 catalyst (Cu NPs of 3.8 nm, Cu loading of 55.89 wt%, oxygen vacancies of 2.316 × 10 15 spins g −1 ) exhibited an excellent H 2 evolution rate of 58.39 μmolg cat −1 s −1 even at low temperature of 210 °C, which was 2.1-fold enhancement than that of commercial Cu/ZnO/Al 2 O 3 catalyst. Characterizations and experiments revealed that ZnO/CeO 2 intensified the strong metal-support interaction (SMSI), which anchored the Cu NPs, generated abundant oxygen vacancies and adjusted electronic structure to form Cu 0 -Cu + -O v active sites for facilitating the kinetics of APRM.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Yinhe Hai,Tong Guan,Yibin Feng,Ziheng Zhen,Youwei Yang,Ying Hu,Jing Lv,Yue Wang,Xinbin Ma
A promising route for producing biodegradable polyglycolic acid material from syngas has garnered increasing attentions. In this route, one of the pivotal issues is developing favorable catalysts for semi-hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG). Silver catalysts were reported to be effective but suffered from the high cost. Herein, we prepared small-sized Cu@Ag/SiO 2 catalysts with appropriate Ag/Cu ratios by a facile wet impregnation method. This core–shell structure facilitated the intermetallic electronic transference from Cu to Ag. The surface exposure of electron-rich silver species could promote the catalytic activity and MG desorption in the DMO hydrogenation, which achieved high efficiency without compromising the MG selectivity. The optimal catalyst with Ag/Cu mass ratio of 3/2 displayed excellent space time yield towards MG of 47.3 g·g Ag −1 ·h −1 . These insights could offer a potential strategy to reduce the silver-based catalyst cost for the semi-hydrogenation of DMO to MG.
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
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2024
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IF 6.1
Tao Liu,Chang Jiang,Zekai Liu,Xuehui Zhang,Wenmin Zhao,Longfei Zeng,Lina Zhang
Reduced graphene oxide (rGO) with surface-loaded Cu particles (scCu-rGO) was prepared by supercritical CO 2 deposition, and Cu matrix composites with scCu-rGO as a reinforcement (scCu-rGO/Cu composites) were successfully prepared by ball milling for different times and spark plasma sintering (SPS). The scCu-rGO/Cu composites prepared with a ball milling time of 20 h exhibited high electrical conductivity (96.3 % IACS), tensile strength (240 MPa), and elongation (37 %). The outstanding properties are mainly ascribed to the uniform distribution of rGO by the ball milling process and rGO promoted by loading Cu particles onto its surface through supercritical deposition, which led to an interfacial reaction between rGO and Cu, resulting in the formation of a Cu 2 O transition layer with a load-transferring effect that enhanced the mechanical properties of the composites. Based on the experimental results, the strength of scCu-rGO/Cu composites is mainly enhanced by synergistic strengthening through grain refinement, Orowan looping and load transfer strengthening. This study demonstrates that the use of supercritical deposition to construct Cu 2 O transition layers can result in a strength-plasticity and high electrical conductivity match in scCu-rGO/Cu composites. The findings presented here offer new insights for innovative design of Cu matrix composites for advanced engineering applications by using supercritical deposition.
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CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Junjie Xu,Wei Sun,Xiang Xiong,Hongbo Zhang,Lingkun Yang
Spacecraft thermal protection materials need to survive long-term exposure to oxygen-containing environments at 2400 °C. In this study, a high-density and low-porosity metal-ceramic-modified composite was prepared at a low temperature (1500 °C) in the presence of W and Cu using combined slurry brushing and reactive melt infiltration methods. An investigation of the composite formation mechanism and the effects of W and Cu indicated that W and ZrB 2 were formed via dissolution-precipitation and the external diffusion of C and B, respectively. The low reaction temperature and the metallic phases significantly improved the mechanical properties, thermophysical properties, and long-term ablation behaviours of C/C–ZrC–ZrB 2 –W–Cu. Compared to traditional C/C–ZrC, the flexural strength and fracture toughness of the composite increased by 71.56 % and 90.05 % to 345.95 MPa and 14.52 MPa m 1/2 , respectively, and the thermal conductivity increased by 174.93 % to 59.11 W/m·K. In addition, W and Cu effectively lowered the surface temperature by nearly 250 °C during 300 s ablation, and the mass and line ablation rates decreased to −0.272 mg/s and −0.247 μm/s, respectively.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3369-3389
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IF 2.8
Wang Lu,Rehman Mooeez ur,Jiang Yong,Sun Fan,Zhao Yuanqi,Lu Xiyue,Zhang Zhijun,Liu Wei,Xu Yan,Zhai Yong,Zhao Yujun
With the growing global demand for biodegradable plastics, the hydrogenation of dimethyl maleate (DMM) to produce 1,4-butanediol (BDO), raw materials for poly(butylene succinate), has become one of the hot spots in chemical industry. In this work, we synthesized a series of Cu@C/ZnO–S x catalysts by the method of sorbitol modification for the liquid-phase hydrogenation of DMM. The modification with appropriate sorbitol led to a decoration of carbon on catalyst surface, which improved the copper dispersion and Cu + /(Cu 0 + Cu + ) molar ratio in the Cu@C/ZnO–S 0.08 catalyst. The carbon decoration not only promoted the formation of more copper species having stronger interaction with ZnO, but also enhanced the absorption of ester on catalyst surface. These distinctive properties contributed to the high performance of the Cu@C/ZnO–S 0.08 catalyst in DMM hydrogenation, achieving an excellent BDO yield of 98.4% and superior reusability. The insights into the roles of sorbitol modification could give valuable guidance to the further design of high performance catalysts for esters hydrogenation. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiaxin Luo,Yang Qin,Dongbin Zhang,Tong Dou,Meina Tan,Fazhi Zhang,Xuhui Zhao,Yiping Wang,Lirong Zheng,Xiaodong Lei
Due to the modification of anions, an electron redistribution occurs at the metal ions can affect the electronic structure, and induce excellent specific capacity. Herein, we report an effective and low time-consuming method by in-situ wet chemical reduction at room temperature to construct S-modified Cu/Cu 2 O negative electrode material. Moreover, the sulfur can occupy partial O sites in Cu 2 O to play a crucial role in the electronic structure of the material, demonstrated by DFT calculation, XRD, XPS and XAS measurements. The prepared S-Cu/Cu 2 O samples exhibit excellent electrochemical performance with high specific capacity of 669 mAh·g −1 at 1 A·g −1 , even 450 mAh·g −1 at 10 A·g −1 . When the materials are composed as pseudo capacity-type cathode//battery-like anode (MnO 2 //S-Cu/Cu 2 O), and (+) battery-type//battery-type (-) (Ni-Cu hydroxide/Cu(OH) 2 /CF//S-Cu/Cu 2 O) hybrid capacitors, they show the energy density of 47.7 and 147.3 Wh·kg −1 at the power density of 636.2 and 800 kW·kg −1 , respectively. Otherwise, the flexible MnO 2 //S-Cu/Cu 2 O hybrid capacitor is assembled, which also exhibits good performance at different bending conditions. This work can provide a simple method to prepare the electrode materials via in situ anion modification for high-energy density battery-like energy storage systems.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Xiangyu Wang,Yubing Sun,Qiang Wang,Lijun Tang,Hui Wang,Tiansheng Mu,Yongchao Zhang,Xiaodong Zhu,Jian Gao
Three-dimensional (3D) carbon materials are often used as carriers for anchoring iodine in zinc-iodine batteries (ZIBs). However, the physical stacking of carbon materials during the electrode assembly process, the weaker physical interactions between non-polar carbon materials and iodine species, and the scarcity of catalytic sites for iodine conversion led to a reduced catalytic activity for the iodine redox reaction, which fails to completely inhibit the shuttling of iodine species. Here, 3D ultrafine Cu-anchored CNT-rGO carriers (3D Cu@CNT-rGO) with interconnected structures are prepared using a simple laser-induced reduction strategy. The 3D microporous structure and excellent electrical conductivity of 3D Cu@CNT-rGO make it an ideal host for iodine. Ultrafine Cu nanoparticles introduce as catalysts accelerate the redox kinetics, efficiently catalyze iodine/polyiodide conversion, inhibit polyiodide shuttling, and enhance the electrochemical performance of ZIBs. The fabricated zinc-iodide micro-batteries (ZIMBs) delivers a high specific area capacity of 1.29 mAh cm −2 , a high area energy density (1.55 mWh cm −2 ) and a high area power density (33.58 mW cm −2 ) as well as excellent cyclin stability (80% capacity retention after 4000 cycles). Meanwhile, ZIMBs have excellent mechanical flexibility and have great potential for application in the field of integrated, miniaturized and flexible electronic devices.
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ANALYTICA CHIMICA ACTA
·
2025
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IF 6
Xing Zhong,Hezheng Zhan,Xiao Wang,Min Zhang,Shoushan Wang,Meili Zhang,Faliang Cheng,Peng Liu
Background Surface-enhanced Raman spectroscopy (SERS) substrates have undergone extensive development over the years, yet the challenge of significantly enhancing their sensitivity persists. Most existing substrates face considerable difficulties in obtaining the strongest electromagnetic coupling to maximize SERS signal intensity, i.e., it is hard to achieve optimal structural parameters such as the gap width and particle size, and to fabricate surfaces that are free from contamination such as surfactants. Therefore, there is a pressing need for a substrate optimization approach that allows for in-situ monitoring and real-time dynamic adjustments to precisely achieve the ideal substrate characteristics for superior performance. Results In this study, a highly sensitive porous copper-gold (Cu–Au) SERS substrate was fabricated using the galvanic replacement reaction (GRR), coupled with in-situ SERS monitoring to optimize substrate preparation. The Cu–Au nanoparticles formed and grew on sacrificial templates while noble metal ions were reduced by the sacrificial metal during GRR. The substrate preparation process revealed that the optimal preparation time was 200 ± 20 s. The SERS performance with crystal violet (CV) as a probe molecule demonstrated the substrate's remarkable sensitivity with detecting concentrations as low as 10 −16 M, which surpasses most literature reports. The optimized SERS substrate was further tested for detecting malachite green (MG), yielding an ultra-high enhancement factor (EF) of 8.96 × 10 14 . The entire optimization process did not involve the addition of aggregation or surfactant agents, ensuring a clean substrate surface. Significance and novelty This study is a further proof of the significance of the in-situ optimization of SERS substrates via GRR which allows real-time adjustment of nanoparticle size and gap width to enhance sensitivity. This approach has enabled us to develop substrates with exceptional sensitivity and reproducibility. These significant contributions may open up new avenues for the facile fabrication of ultrasensitive SERS substrates.
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Applied Sciences-Basel
·
2024
·Vol. 14
·期 18
·8285
·
IF 2.5
Yihang Liu,Zongmao Lu,Jiajie Wang,Jinghui Lai,Ziyang Li,Chu Zhang,Yuhang Qi
Cu interconnect chemical mechanical polishing (CMP) technology has been continuously evolving, leading to increasingly stringent post-CMP cleaning requirements. To address the environmental pollution caused by traditional post-CMP cleaning solutions, we have explored the use of photocatalytic processes to remove citric acid, which is a commonly used complexing agent for CMP. In this study, CeO2abrasives, characterized by a hardness of 5.5, are extensively employed in CMP. Importantly, CeO2also exhibits a suitable band structure with a band gap of 2.27 eV, enabling it to photocatalytically remove citric acid, a commonly used complexing agent in Cu CMP. Additionally, the integration of H2O2, an essential oxidant in Cu CMP, enhances the photocatalytic degradation efficiency. The research indicates that the removal rate of single-phase CeO2was 1.78 mmol/g/h and the degradation efficiency increased by 40% with the addition of H2O2, attributed to the hydroxyl radicals generated from a Fenton-like reaction between H2O2and CeO2. These findings highlight the potential of photocatalytic processes to improve organic contaminant removal in post-CMP cleaning, offering a more sustainable alternative to conventional practices.
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