CRYSTENGCOMM
·
2024
·Vol. 26
·期 48
·6844-6851
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IF 2.6
Yuyuan Chen,Yachang Huang,Xia Hu,Sijie Lin,De-Kun Ma
The exposed crystal facets of Cu have a profound effect on its electrocatalytic CO2 reduction reaction (CO2RR) activity and product selectivity. On the other hand, at present, most of the studies on Cu-based electrocatalysts for the CO2RR focus on the synthesis of C2+ products. There are only a few reports involving methanol (CH3OH) generation over Cu nanocrystals. Herein, CuO nanosheets (NSs) and nanorods (NRs) were synthesized through a controlled oxidation and dehydration route under mild reaction conditions, using Cu mesh as a Cu source and conductive substrate, respectively. The as-synthesized CuO NSs and NRs were further converted into Cu NSs and NRs through an in situ electrochemical reduction method, respectively. The experimental results showed that CH3OH could be efficiently produced over Cu NSs with abundant (111) crystal facets through the electrocatalytic CO2RR. The maximum CH3OH faradaic efficiency (FE) obtained on Cu NSs is 68% at a relatively low applied potential of −0.6 V vs. reversible hydrogen electrode (RHE), which is 1.6 times larger than that achieved on Cu NRs with primarily exposed (200) crystal facets (42%). The crystal facet-dependent electrocatalytic CO2RR activity toward CH3OH production was elucidated based on theoretical calculations combined with experimental results.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
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 Materials & Interfaces
·
2024
·
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
·
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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ACS Applied Polymer Materials
·
2024
·
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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CHEMICAL ENGINEERING SCIENCE
·
2024
·
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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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
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
·
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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CHEMICAL ENGINEERING JOURNAL
·
2024
·
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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RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3369-3389
·
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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LANGMUIR
·
2024
·
IF 3.7
Yun-Long Mu,Qing He,Chun-Yan Li,Da Sheng,Song-Hai Wu,Yong Liu,Hai-Tao Ren,Xu Han
Although precise regulation of the crystalline structures of metal oxides is an effective method to improve their antibacterial activities, the corresponding mechanisms involved in this process are still unclear. In this study, three kinds of cuprous oxide (Cu2O) samples with different structures of cubes, octahedra, and rhombic dodecahedra (c-Cu2O, o-Cu2O, and r-Cu2O) have been successfully synthesized and their antibacterial activities are compared. The antibacterial activities follow the order of r-Cu2O > o-Cu2O > c-Cu2O, revealing the significant dependence of the antibacterial activities on the crystalline structures of Cu2O. Quenching experiments, as well as the NBT and DPD experiments indicate that ≡CuII─OO• superoxo and ≡CuII─OOH peroxo, instead of •OH, O2•–, and H2O2, are the primary oxidizing species in the oxidative damage to E. coli. Raman analysis further confirms the presence of both ≡CuII─OO• superoxo and ≡CuII─OOH peroxo on the surface of r-Cu2O. On the other hand, the NCP experiment reveals that Cu+, instead of Cu2+, also contributes to the antibacterial process. This study provides new insight into the antibacterial mechanisms of Cu2O.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Junfeng Kong,Huazhen Cao,Weilun Qian,Lining Yu,Anyang Tang,Wenyu Feng,Huibin Zhang,Guoqu Zheng
Arsenic is a harmful associated element in antimony ore, which might bring out the risk of leakage during complex industrial production of high-purity antimony. Herein, we reported a novel and efficient way to remove the trace arsenic impurity from acidic SbCl 3 solution by utilizing copper-system bimetallic particles. Specifically, galvanically coupled Cu 2 Sb/Cu was in-situ synthesized by introducing precursor copper powder to the specific SbCl 3 solution. DFT studies revealed that Sb(III) was easily reduced by Cu to form Cu 2 Sb due to the strong adsorption of Sb(III) on Cu (111) crystal plane. The Cu 2 Sb/Cu coupling exhibited excellent activity for As(III) reduction, over 99.4% arsenic were removed under optimal conditions and residual arsenic concentration dropped to only 2.7 mg L −1 . Crucially, Sb(III) concentration changes could be neglected. Besides, the dearsenization residues were extensively characterized to analyze the evolvement and cause in the reaction process. The results confirmed that the arsenic removal mechanisms by Cu 2 Sb/Cu particles were multi-affected, including adsorption, displacement, and precipitation. And the strong electrostatic attraction of AsO + under high HCl conditions was identified as a key step to achieving dearsenization. This research will provide a theoretical guidance for the green synthesis of high-purity antimony and related products.
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