Catalysts
·
2025
·Vol. 15
·期 5
·455
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IF 4
Wenjun Lei,Yan Fu,Shipeng Gu,Shuaishuai Qiu,Jie Chang
Catalytic hydrogenolysis of lignin to produce high-value monophenols has emerged as a pivotal strategy in modern biorefineries. In this study, we synthesized spherical nitrogen-doped porous carbon (SNCB) materials by using Al/Co-BTC as a precursor, introducing melamine as a supplementary carbon and nitrogen source, and activating the material with NaOH solution. The SNCB framework was decorated with Cu-Pd bimetallic nanoparticles, exhibiting outstanding catalytic activity in the hydrogenolytic depolymerization of organosolv lignin. The Cu-Pd@SNCB catalyst exhibited remarkable activity, attributed to the hierarchical porous structure of SNCB that facilitated metal nanoparticle dispersion and reactant accessibility. The synergistic effect between Cu as the reactive site for reactant adsorption and Pd as the reactive site for H2adsorption enhanced the catalytic activity of the catalyst. Systematically optimized conditions (2 MPa H2, 270 °C, 3 h) yielded 43.02 wt% phenolic monomers, with 4-(3-hydroxypropyl)-2,6-dimethoxyphenol dominating the product profile at 46.3% selectivity. The catalyst and its reaction products were analyzed using advanced characterization techniques, including XPS, XRD, TEM, SEM, BET, GC-MS, GPC, 2D HSQC NMR, and FT-IR, to elucidate the reaction mechanism. The mechanism proceeds through: (1) nucleophilic substitution of the β-O-4 hydroxyl group by MeOH, followed by (2) simultaneous hydrogenolytic cleavage of Cβ-O and Cα-O bonds mediated by Cu-Pd@SNCB under H2atmosphere, which selectively produces 4-(3-hydroxypropyl)-2,6-dimethoxyphenol and 4-propyl-2,6-dimethoxyphenol. This study proposes a bimetallic synergistic mechanism, offering a general blueprint for developing selective lignin valorization catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kang Feng,Jing Cao,Dandan Wu,Jianan Li,Qi Zuo,Shaojun Bai
This study investigates the effect of sodium percarbonate (SPC) as an eco-friendly oxidant on the flotation separation of bornite and arsenopyrite. Micro-flotation tests demonstrated that SPC significantly suppressed arsenopyrite floatability while maintaining bornite floatability. In artificial mixed-ore tests conducted at pH 10 with 500 mg/L SPC and 5 × 10 −5 mol/L sodium butyl xanthate (NaBX), bornite recovery reached 87.93 %, whereas arsenopyrite recovery was only 14.51 %, which resulted in a substantial recovery difference of 73.42 %. Surface analysis via contact angle measurements, scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), atomic force microscopy (AFM), localized electrochemical impedance spectroscopy (LEIS), X-ray photoelectron spectroscopy (XPS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) revealed that SPC treatment enhanced the hydrophilicity of arsenopyrite compared with that of bornite. LEIS, XPS, and ToF-SIMS confirmed the formation of hydrophilic oxides such as FeAsO 4 , H 3 AsO 3 , Fe(OH) 3 , and Fe 2 (SO 4 ) 3 on arsenopyrite surfaces, which ultimately reduced floatability. In contrast, bornite surfaces exhibited only slight oxidation, with minimal increases in Cu(OH) 2 , Fe(OH) 3 , and Fe 2 (SO 4 ) 3 which only resulted in a modest decrease in floatability. SEM–EDS and AFM analyses revealed significant changes in the surface morphology of arsenopyrite after SPC treatment, with increased oxygen content and surface roughness, which indicated the formation of an oxide layer. In contrast, bornite surfaces remained relatively smooth, with only a slight increase in oxygen content. This study provides valuable theoretical reference into the use of eco-friendly depressants for copper–arsenic mineral separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haining Hou,Zehao Zhang,Haibo Li
Capacitive deionization (CDI) is a highly efficient desalination technique to obtain the portable water with low energy cost and environmental-friendly. However, the desalination capacity is still challenging. In this work, a Cu@C anode presenting the spherical structure with plenty of 3D diffusion tunnels has been proposed for CDI anode towards the enhanced Cl - removal. Such structure not only provide abundant electroactive sites for adopting salty ions, but also promote the electrosorption kinetics. Aiming to extract Cl - from the stream, the optimized Cu@C // activated carbon CDI device demonstrates the exceptional desalination capacity of 149.14 mg/g at 1.4 V in 529 ppm NaCl solutions as well as the fast desalination rate of 8.32 mg/g/min, which are relatively high as compared to many reported data. Moreover, the mechanism analysis points out that the desalination behavior of Cu@C electrode is dominantly governed by the conversion of Cu 0 and Cu + . Beyond that, the desalination capacity decay upon the long cycles is attributed to the irreversible Cu-Cl bonds.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Xinyu Peng,Xiaoxian Zhang,Hongrui Chen,Xiaoran Zhang,Chaohong Tan,Xiaojuan Bai,Yongwei Gong,Yang Qu,Haiyan Li,Ziyang Zhang
In recent years, the escalating attention on Pharmaceutical and Personal Care Products (PPCPs) and Heavy Metals in urban stormwater runoff highlights the critical role of Road-deposited sediments (RDS) as a significant carrier for pollutant occurrence and transport in runoff. However, existing research has overlooked the composite characteristics of PPCPs and Heavy Metals, hampering a holistic understanding of their transformation in diverse forms within runoff. This limitation impedes the exploration of their subsequent migration and conversion properties, thereby obstructing coordinated strategies for the control of co-pollution in runoff. This study focuses on the typical PPCP sulfamethoxazole (SMX) and heavy metal Cu(II) to analyze their occurrence characteristics in the Runoff-RDS system. Kinetics and isotherm studies reveal that RDS effectively accumulates SMX and Cu(II), with both exhibiting rapid association with RDS in the early stages of runoff. The accumulation of SMX and Cu(II) accounts for over 80 % and 70 % of the total accumulation within the first 240 min and 60 min, respectively. Moreover, as runoff pH values decrease, the initially synergistic effect between the co-pollutant transforms into an antagonistic effect. In the composite system, varying pH values from 2.0 to 6.0 lead to an increase in SMX accumulation from 4.01 mg/kg to 6.19 mg/kg and Cu(II) accumulation from 0.43 mg/g to 3.39 mg/g. Compared to the single system, the composite system capacity for SMX and Cu(II) increases by 0.04 mg/kg and 0.33 mg/g at pH 4.0. However, at pH 3.0, the composite system capacity for SMX and Cu(II) decreases by 0.21 mg/kg and 0.36 mg/g, respectively. Protonation/deprotonation of SMX under different pH conditions influences electrostatic repulsion/attraction between SMX and RDS. The mechanism of RDS accumulation of SMX involves Electron Donor-Acceptor (EDA) interaction, hydrogen bond interaction, and Lewis acid-base interaction. Cu(II) enrichment on RDS includes surface complexation reaction, electrostatic interaction, and surface precipitation. Complex formation enhances the accumulation of both SMX and Cu(II) on RDS in runoff. This study elucidates the co-occurrence characteristics and mechanisms of SMX and Cu(II) co-pollution in runoff systems. The findings contribute valuable insights to understanding the existence patterns and mechanisms of co-pollution, providing a reference for investigating the migration and fate of co-pollutant in runoff. Moreover, these insights could offer guidance for the development of effective strategies to mitigate co-pollution in rainwater.
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DIAMOND AND RELATED MATERIALS
·
2024
·
IF 4.3
Zhen Li,Xianhui Wang,Da Li,Hongbo Zhang,Bochen Zhang
The Mo 2 C@CNTs/Cu-20wt.%Mo composite materials with outstanding mechanical properties and electrical conductivity were prepared via the combination of mechanical wet-mixing, ball-milling and spark plasma sintering technology. By regulating the morphology and content of Mo 2 C decorated on CNTs, the Mo 2 C nanoparticles are anchored on CNTs and well bonded with the matrix, resulting the good interfacial bonding in the composite material. The Cu-20wt.%Mo composite material reinforced by 0.2wt.%Mo 2 C@CNTs exhibits a yield strength of 342.19 MPa and an ultimate tensile strength of 390.37 MPa, which are respectively increased by 23.13 % and 20.34 % as compared to the Cu-20wt.%Mo. Besides, the electrical conductivity of the 0.2wt.%Mo 2 C@CNTs/Cu-20wt.%Mo composite material is also improved by 6.89 %. Furthermore, the strengthening effect of Mo 2 C@CNTs/Cu-20wt.%Mo composite material can be attributed to the contribution of Mo 2 C nanoparticles, which not only enhance the CNTs load transfer strengthening but also promote the dislocation strengthening and Orowan strengthening.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Shujun Huang,Xinyan Chen,Yu Lei,Wanting Zhao,Jipeng Yan,Jian Sun
Laccase is a very promising natural enzyme in the application of biochemical industry, but its application is severely limited by its high cost and poor stability. To overcome the inherent defects of natural laccase, here, we prepared a new type of small-size mimicking nanozymes based on self-assembly of bovine serum albumin (BSA) and copper sulfate (CuSO 4 ) with help of ionic liquid (IL). The effects of different ILs on the catalytic activity of the product (BSA-Cu nanozymes) were investigated, and it was found that BSA-Cu nanozymes with stable structures could be obtained in tetrabutylammonium hydroxide (TBAOH). Compared with laccase, the V max /K m of BSA-Cu nanozymes prepared by TBAOH was higher (0.081) than that of laccase (0.029), and the stability of BSA-Cu nanozymes were significantly enhanced in terms of pH, temperature, and ionic strength. The BSA-Cu nanozymes were utilized for detection and degradation of a series of phenolic substances, among which catechol was the most effective. In the detection of epinephrine, BSA-Cu nanozymes achieved a lower detection limit (0.38 µg/mL) and were more sensitive than laccase (3.53 µg/mL). The application of ILs can improve the mimicking laccase nanozymes performance and has great potential for further industrial application.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Dandan Hu,Tianyu Zhan,Zhiyong Guo,Sui Wang,Yufang Hu
A novel dual-modality readout biosensing method is developed for Cu(II), coenzyme (CoA) and histone acetyltransferase (HAT) analysis based on an electrosynthesized tris(bipyridine)ruthenium(II)-functionalized metal-organic framework (Ru-MOF). In this protocol, the Ru-MOF with a delicate structure serves as both an electrochemiluminescent (ECL) and fluorescent (FL) probe. Interestingly, Cu(II) can hinder the two distinct processes favorably, thus realizing bidirectional detection of Cu(II) via an “on-off” method. Simultaneously, CoA, which contains a sulfhydryl group, can ignite a reverse “off-on” process due to the polymeric interaction of CoA and Cu(II) (2: 1). Similarly, abundant CoA molecules could also be generated regularly by a typical HAT p300-driven acetylation reaction, hence accomplishing HAT p300 activity analysis. Subsequently, an ingenious “on-off” route is exhibited again by the introduction of some small molecules (including anacardic acid and C646), which present an inhibiting effect on HAT p300 activity. Furthermore, quantitative analysis of Cu(II), CoA and HAT p300 (ECL/FL) is achieved brightly with detection limits of 0.19/0.76 nM, 1.3/6.5 nM and 1.5/8.8 nM, respectively. Ultimately, this two-channel biosensor with excellent analytical performance is applied successfully in real samples, demonstrating its potential use in bioanalysis.
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Small
·
2025
·
IF 12.1
Fukang Feng,Xiaoyu Zhang,Xinrui Han,Guangyu Wu,Weinan Xing
The efficiency of peroxymonosulfate (PMS) activation in photocatalytic processes critically depends on the regulation of electron transfer from generation to utilization. Herein, a holistic electron transfer pathway is constructed within a metal–organic frameworks (MOFs)-derived Cu-Cu x O/TiO 2 composite to achieve superior PMS activation. The incorporated Cu species serve as dynamic redox mediators, enabling an efficient non-photoinduced electron transfer pathway via Cu 0 &Cu n+ cycling. Simultaneously, the Cu-induced bandgap narrowing and abundant oxygen vacancies significantly enhance visible-light absorption and facilitate the rapid trapping of photogenerated electrons. This synergy establishes a continuous and highly efficient electron transfer from photoexcitation to catalytic reaction. The optimized catalyst Cu-Cu x O/TiO 2 -2 delivers an exceptional tetracycline hydrochloride (TC) degradation rate constant of 38.26 × 10 −3 min −1 , representing a 2.04-fold enhancement over pristine TiO 2 (18.74 × 10 −3 min −1 ). Mechanistic studies confirm that the radical ( • OH/ • SO 4 − ) and non-radical (h⁺) pathways function synergistically in the Cu-Cu x O/TiO 2 -2/PMS system, collectively enabling highly efficient TC degradation. Three plausible degradation routes are proposed based on intermediates identification and density functional theory (DFT) calculations. Furthermore, economic analysis is conducted to transition from mechanistic insight to practical value, assessing the commercial potential of the Cu-Cu x O/TiO 2 -2/PMS photodegradation system. This work provides valuable insights into the design of efficient composite catalysts through regulated electron transfer via dynamic redox cycling coupled with oxygen vacancy engineering.
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Advanced Science
·
2025
·
IF 14.1
Chuanlong Men,Chenchen Wu,Lei Wang,Shengjie Gao,Yu Mao,Wei Liu,Changhong Liu,Lei Zheng
Postharvest preservation urgently demands innovative solutions bridging atomic precision with practical scalability. Here, a distinctive photocatalysis-driven self-assembly strategy is presented that fundamentally diverged from conventional high-temperature syntheses by enabling precise single-atom coordination under ambient conditions. This approach, utilizing α-lipoic acid (α-LA) as coordination ligand, achieved the mild assembly of S-coordinated Cu single-atom nanozymes (Cu/CNS) while significantly enhancing their enzymatic activity. The resulting material demonstrated unprecedented multi-enzyme mimetic activities (catalase-, oxidase-, and glutathione oxidase-like) with catalytic efficiency surpassing conventional nanozymes by orders of magnitude. The Cu/CNS exhibits near-perfect antimicrobial efficacy against Escherichia coli ( E. coli ), Staphylococcus aureus ( S. aureus ), and Botrytis cinerea ( B. cinerea ) through synergistic mechanisms. When integrated into chitosan-gelatin films (Cu/CNS@CS-Gel), it forms active packaging with pH-responsive behavior, exceptional barrier properties, and mechanical strength. Crucially, the synthesis is simple, scalable, and environmentally adaptable. Using strawberries and kiwifruits as representative examples, Cu/CNS@CS-Gel more than doubled the shelf life while efficiently maintaining nutritional quality. Beyond food packaging, this coordination chemistry platform is generalizable to other metal-ligand systems, offering a versatile toolbox for sustainable agriculture. By bridging atomic-level design with practical feasibility, the work advances sustainable nanozyme implementation in food systems.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Zhixuan Tan,Bin Liang,Jiaping Yang,Kepan Yan,Jiarong Chen,Xiaoying Liu,Xu Peng,Tangchao Xie,Yijuan Li
Zinc metal is one of the most promising anode materials for aqueous batteries. However, nonuniform deposition of zinc metal anodes and hydrogen evolution reactions (HER) severely affect the stability of aqueous zinc–ion batteries. Herein, a simple redox reaction between zinc metal and graphene oxide and a subsequent one-step replacement reaction were utilized to in situ fabricate rod-shaped zinc oxide, reduced graphene oxide (rGO), and Cu nanoparticles on the zinc anode surface. This ingenious design constructs an artificial gradient zinc-affinity interface layer (ZnO–rGO–Cu), which regulates the longitudinal electric field distribution, enabling Zn2+ to deposit uniformly along the gradient from bottom to top, thereby suppressing the dendrites growth. Besides, Cu nanoparticles and rGO partially isolate the zinc from the electrolyte to inhibit the unwanted HER. Moreover, these components reduce the interface contact angle with aqueous electrolytes, enhancing electrolyte affinity and electrochemical activity. Consequently, the Zn–rGO–Cu symmetric cells cycle stably for 1000 h at 1 mA cm–2, and the half-cells achieve 1500 stable cycles at 2 mA cm–2 with a high Coulombic efficiency of 99%. Furthermore, full cells paired with manganese-based and vanadium-based cathodes stably cycle 900 times at 0.5 A g–1 and 600 times at 2 A g–1, respectively. This study thus provides insights into rationally designing multifunctional interphase layers for high-performance zinc–ion batteries.
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RARE METALS
·
2025
·
IF 11
Taichong Chitboonyakasem,Ya Gao,Xinbo Qiu,Jing Peng,Jian Zhou
en The sluggish kinetics of the oxygen reduction reaction (ORR) necessitate developing oxygen electrodes with enhanced electrocatalytic activity for practical zinc–air battery applications. In this study, an iron-doped copper sulfide electrocatalyst (CuFeNS-PNC) anchored on metal–organic framework-derived carbon substrates was designed, featuring a bimetallic Cu 5 FeS 4 architecture where iron electronically modulates copper sites. The performance enhancement of this copper–iron sulfide bimetallic system relative to a monometallic copper sulfide arises from synergistic Fe-Cu interactions, as confirmed by X-ray photoelectron spectroscopy (XPS), revealing electron transfer from iron to copper. Density functional theory (DFT) calculations demonstrate that iron incorporation downshifts the copper d-band center, weakening OH* adsorption energy to a more optimal level, thereby boosting ORR kinetics. Consequently, the CuFeNS-PNC catalyst achieves superior electrocatalytic performance with an ORR onset potential ( E onset ) of 0.988 V and a half-wave potential ( E 1/2 ) of 0.874 V, significantly surpassing commercial Pt/C and conventional metallic sulfide catalysts. When integrated into a zinc–air battery, it delivers a high open-circuit voltage (1.450 V), specific capacity (789 mAh g −1 ), and peak power density (117.9 mW cm −2 ). This work provides valuable guidelines for the rational design and synthesis of electronically modulated metallic sulfides to enhance ORR activity for energy storage and conversion applications. 摘要 zh 氧还原反应 (ORR) 的缓慢动力学过程限制了锌空气电池的实际应用, 因此开发具有优异电催化活性的氧电极材料至关重要。本研究设计了一种负载于金属有机框架衍生碳基底上的铁掺杂铜硫化物电催化剂 (CuFeNS-PNC) , 其结构为双金属Cu 5 FeS 4 , 其中铁元素通过电子调控作用调节铜活性位点。与单金属铜硫化物相比, 该双金属体系的性能提升源于Fe–Cu之间的协同作用。X射线光电子能谱结果表明, 存在从Fe向Cu的电子转移。密度泛函理论计算进一步揭示, 铁的引入使铜的d带中心下移, 优化OH*的结合强度, 进而加速ORR动力学过程。因此, CuFeNS-PNC催化剂表现出优异的电催化性能, 具有0.988 V的氧还原起始电位和0.874 V的半波电位, 显著优于商用Pt/C及常规金属硫化物催化剂。应用于锌空气电池时, 该催化剂实现了高达1.450 V的开路电压、789 mAh g⁻ 1 的比容量以及117.9 mW cm⁻²的峰值功率密度。本研究为通过电子结构调控设计高效金属硫化物催化剂以提升氧还原活性、促进能量存储与转换应用提供了有价值的指导。
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Catalysis Science & Technology
·
2025
·
IF 4.2
Yumei Zhang,Yue Wang,Dongle Wang,Yating Liu,Tong Gao,Qingqiang Zhou,Qingzhi Luo,Jing An,Xueyan Li,Yandong Duan,Desong Wang
A novel Cu–B2O3/porous boron nitride (PBN) composite was developed as a highly efficient and reusable heterogeneous catalyst for the solvent-controlled conversion of arylboronic acids. In water, the catalyst promotes ipso-hydroxylation to phenols, while in methanol, it facilitates aerobic homocoupling to biphenyls, using air as a green oxidant. The synergistic interaction between Cu nanoparticles and B2O3 sites enhances both catalytic activity and stability. This work offers a sustainable and selective approach for synthesizing phenolic and biphenyl compounds under mild conditions.
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