INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
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IF 9.2
Jiaoyan Li,Tianyu Li,Kun Sun,Junhao Chang,Peng Zheng,Yajing Zhang,Fangke Wang,Kangjun Wang
EMSI enhances FFA ring-opening hydrogenolysis to 1,2-PeD. • Electron-deficient Cu species and basic sites synergistically activate C–O bonds. • In situ ATR-FTIR reveals furan-ring opening and C 5 intermediate formation. • DFT reveals furan-O adsorption promotes C 5 –O 1 bond polarization and cleavage. Selective hydrogenolysis of furfuryl alcohol (FFA) to 1,2-pentanediol (1,2-PeD) offers a route for biomass valorization. However, catalysts suffer from unclear active-site configurations and insufficient activation of the key C–O bond. To address this, a Cu/MgO catalyst featuring basic sites and electron-deficient Cu active sites at the interface is developed. Compared with Cu/Al 2 O 3 and Cu/CeO 2 , Cu/MgO achieves 97% FFA conversion and 45% 1,2-PeD selectivity under continuous-flow conditions at 140 °C and 6 MPa H 2 . In situ XPS, in situ ATR-FTIR, and DFT calculations indicate that electronic metal-support interaction (EMSI) at the Cu–MgO interface induces interfacial charge redistribution and favors ring-opening hydrogenolysis. The resulting electron-deficient Cu species and MgO-derived basic sites cooperatively promote FFA adsorption through the furan-ring oxygen, C–O bond activation, C 5 carbonyl intermediate formation, and hydrogenation to 1,2-PeD. This work addresses the mechanistic gap between EMSI and the ring-opening hydrogenolysis of FFA over Cu–MgO catalysts. Cu–MgO interfacial sites, where EMSI generates electron-deficient Cu species while MgO provides basic sites, enable selective ring-opening hydrogenolysis of furfuryl alcohol to 1,2-pentanediol. Preferential adsorption through the furan-ring O atom positions the C 5 –O 1 bond near the Cu–MgO interface, promoting interfacial polarization, selective C–O bond cleavage, C 5 carbonyl intermediate formation, and subsequent hydrogenation to 1,2-pentanediol, as supported by in situ XPS, in situ ATR-FTIR, and DFT calculations. Download: Download high-res image (331KB) Download: Download full-size image
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2026
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IF 7.9
Shihao Bai,Weijiao Jiang,Jingke Pei,Zhihui Xie,Jian Kang,Ming Xiang,Yue Zhang,Lu Li
High-permeance nanofiltration (NF) membranes with efficient sulfate separation are highly desirable for water purification and ion separation, but their performance is often constrained by the insufficient control of polyamide (PA) formation during interfacial polymerization. Herein, a copper–ionic liquid complex interlayer was constructed in situ on a polysulfone substrate through a coordination-assisted assembly strategy to regulate PA formation and improve NF separation performance. The introduction of the Cu-IL interlayer altered the interfacial polymerization environment, leading to the formation of a thinner and smoother PA selective layer with a modified surface elemental composition. Compared with the pristine NF membrane, the optimized NF/Cu-IL-2 membrane exhibited a reduced PA-layer thickness from 114 to 75 nm, a decreased surface roughness from 9.1 to 7.1 nm, and a lower O/N ratio from 1.22 to 1.13. Benefiting from the reduced transport resistance and improved water affinity, NF/Cu-IL-2 achieved a water permeance of 15.8 L m -2 h -1 bar -1 , which was 85% higher than that of the pristine NF membrane, while maintaining a Na 2 SO 4 rejection above 97%. Notably, the effect of Cu-IL loading was non-monotonic, and further increasing the interlayer loading did not continuously reduce the PA-layer thickness or improve water permeance, indicating the existence of an appropriate Cu-IL loading range. Moreover, NF/Cu-IL-2 maintained relatively stable water permeance and Na 2 SO 4 rejection during a continuous 144 h filtration test under the tested chlorine-free conditions. These results demonstrate that coordination-assisted Cu-IL interlayer engineering is an effective strategy for improving water transport while maintaining sulfate rejection under the investigated single-salt conditions.
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ANALYTICA CHIMICA ACTA
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2025
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IF 6
Rong Huang,Zhong Dong,Wanyi Zhang,Zhenggang Xue,Dongmei Deng,Wei Wang,Yuanyuan Li,Haibo He,Liqiang Luo
Background Organophosphorus pesticides contamination significantly threatens the ecological environment. Therefore, developing sensitive and efficient point-of-care detection methods is essential. Results In this work, Cu−N 4 single-atom nanozymes on nitrogen-doped carbon (Cu SAs/NC) with dual enzyme-mimicking activities (peroxidase-like and oxidase-like) were prepared for point-of-care detection of parathion using acetylcholinesterase inhibition-based colorimetric sensing mechanism. Cu SAs/NC shows high catalytic activity with high turnover number (K cat ) of ∼24.07 min −1 and K cat /K m of ∼1.35×10 5 M −1 min −1 . Experimental findings in combination with density functional theory simulations demonstrate that Cu centers in Cu SAs/NC play a pivotal role in intermediate binding optimization, which contributes to a decreased reaction energy barrier. Hence, a colorimetric sensing platform based on Cu SAs/NC was constructed for point-of-care detection of parathion, achieving a detection limit of 0.79 ng mL −1 . Significance This study provides a novel strategy for structuring single-atom nanozymes with enhanced enzyme-mimicking activity, showing great promise for advanced environmental protection.
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Advanced Healthcare Materials
·
2025
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IF 9.6
Yi Liu,Xujie Cui,Minhao Guo,Jinmei Wu,Yulan Zhao,Guangzheng Zhang,Jiahui Xu,Heyou Han,Weihui Li,Zhiyong Song
Drug-resistant bacterial infections pose a significant threat to global health, creating an urgent need for new antimicrobial agents. Reusing approved drugs has gained attention as a strategy to address this issue. In this study, a nano antibacterial platform (DSF@HKUST-1@Dex) that responds to the infection microenvironment is proposed. This platform releases disulfiram (DSF), binds to copper ions in the mildly acidic conditions of infected areas, converting DSF from nontoxic to toxic in situ, thereby inducing bacterial death and enhancing copper ion absorption. Noncatalytic treatment is also initiated for a synergistic antibacterial effect. Excessive copper ions disrupt bacterial metabolism, inhibit the Tricarboxylic acid (TCA) cycle, reduce ATP levels, and induce cuproptosis-like death, significantly enhancing antibacterial efficacy. In a bacterial wound infection model, the platform exhibited excellent antibacterial activity, promoting wound healing and reducing inflammation. Proteomic analysis showed that the platform selectively targeted bacterial peptidoglycan, disrupted the bacterial cell wall, impacted energy metabolism, and inhibited bacterial growth. In conclusion, this nanoplatform offers a promising strategy for treating drug-resistant infections by repurposing old drugs, converting them to toxic forms, and providing a novel antimicrobial approach.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2026
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IF 3
Wenya Huo,Yike Kuang,Zhendong Sha,Jun Ding
p-Nitrophenol (p-NP) is a toxic and persistent pollutant commonly found in industrial wastewater, necessitating efficient and economically viable treatment strategies. In this work, we develop a low-cost and high-performance catalyst consisting of Fe-Cu-Cr mixed metal oxides supported on activated carbon (AC), synthesized through a simple impregnation-calcination method and applied for peroxymonosulfate (PMS) activation.Systematic optimization of preparation parameters revealed that HCl pretreatment of activated carbon, a ternary Fe-Cu-Cr composition, a 20 wt% metal loading, and calcination at 600 °C yield the highest catalytic activity, achieving p-NP degradation with Ct/C₀ ≈ 0.25 after 4 h. Notably, the total treatment cost can be maintained below 30 CNY per ton of wastewater, demonstrating a substantial economic advantage over reported catalytic systems. Mechanistic studies show that p-NP degradation follows a synergistic adsorption-catalysis pathway, wherein activated carbon enriches p-NP at the catalyst surface and multivalent metal oxides efficiently activate PMS to generate reactive oxygen species, primarily •OH. This work introduces a practical, scalable, and cost-effective catalyst design using earth-abundant metals, offering a promising avenue
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Journal of Materials Chemistry A
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2023
·Vol. 11
·期 12
·6191-6197
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IF 11.9
Hongzhou Yang,He Huang,Qing Wang,Lu Shang,Tierui Zhang,Shouguo Wang
3d transition metal single atom catalysts (SACs) (e.g. M = Fe, Co, Cu) are considered as promising catalysts for oxygen reduction reaction (ORR), among which Fe SACs display comparable performance to commercial Pt/C. However, Fe SACs still demand significant improvements in activity and stability for further industrial deployment. Herein, a Fe, Cu dual metal SAC was synthesized using a facile ligand-mediated method. Fe and Cu atoms were atomically dispersed on commercial carbon black in the form of FeN4 and CuN4 sites. Owing to the interactions between the adjacent Fe and Cu atoms co-existing in a very tiny area, the as-synthesized Fe, Cu dual metal SAC exhibited excellent ORR performance with a high half-wave potential of 0.926 V and good stability in 0.1 M KOH, which are significantly higher than that of the Fe-SAC or Cu-SAC control samples. Density function theory calculations showed that the Cu single atom can act as an electron donator enriching the electron density of Fe sites, thus endowing the Fe sites with optimized adsorption/desorption energy for ORR intermediates and thereby facilitating the ORR activity of FeCu-SAC. Moreover, a study on three typical commercial carbon substrates indicated that carbon support with high surface areas and hierarchical pore structure was beneficial for ORR. The excellent ORR activity and durability of FeCu-SAC enabled the constructed Zn–air battery to have a high power density of 201.4 mW cm−2 and high specific energy of 827.68 W h kg−1.
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RSC Advances
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2023
·Vol. 13
·期 11
·7614-7620
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IF 3.9
Lei Wei,Yanhong Lu,Ruixuan Lu,Yuxin Cui
Hydrolytic dehydrogenation of ammonia borane is a significant and promising approach for on-site hydrogen production at ambient conditions, and developing highly efficient and low-cost catalysts has attracted considerable attention. Herein, waste-biomass-derived activated carbon (AC) was prepared by hydrothermal carbonization and alkali-assisted activation, and non-precious bimetal phosphides (Co–Cu–P) nanocatalysts with a series of different Co/Cu ratios were synthesized on the AC surface through in situ phosphidation method. Owing to the synergetic effects, the optimal Co0.8Cu0.2P/AC presents an outstanding turnover frequency of 26.5 min−1 (25 °C), which is much higher than that of many reported catalysts. The reaction activation energy was measured to be 34.6 kJ mol−1. Benefiting from the ferromagnetic nature of the phosphides, the Co0.8Cu0.2P/AC can be magnetically separated and reused again. After recycling six times, the catalyst still retains 72% of the initial activity, thus indicating great potential for practical applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Shao-Qi Zhi,Jun-Yuan Zhang,Song-Hai Wu,Wen-Shuang Zhu,Yu-Dong Shan,Yong Liu,Xu Han
Turning aromatic sulfur impurities to value-added polymers is a promising technology for fuel desulfurization. In this study, Cu(I,II)@g-C3N4 plates prepared via facile calcination show high reactivity in catalytic oxidation of benzothiophene (BT) by persulfate in a mixture of MeCN/H2O (v/v = 50/50). Quenching experiments rule out the primary contributions of SO4•–, •OH, and O2•– to BT oxidation and confirm the presence of carbon-centered radicals during the desulfurization process. XPS and Raman analyses reveal that Cu(I) and graphitic-N are reactive sites for persulfate activation, accompanied with moderate activation of the peroxo group in persulfate via the nonradical pathway. Solid characterizations indicate the formation of polybenzothiophene S,S-dioxide during the oxidation process, which further reveals that the moderately activated persulfate abstracts H from BT to form a BT radical cation, followed by subsequent polymerization of BT radical cations to a BT tetramer, and then the BT tetramer is further oxidized to a BT S,S-dioxide tetramer. The high electrochemical stability and pseudo-capacitive properties of the obtained polymers also imply their high potential to be used for capacitors. This work provides new insight on turning aromatic sulfur impurities in fuels to “treasures”.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yeshuang Wang,Xuan Liu,Mingxian Duan,Chaonan Zhang,Huiling Fan,Chao Yang,Tingting Jiao,Tian Kou,Ju Shangguan
Isoreticular bimetal M−Cu−BTC has considerable potential in improving the sulfides removal performance of Cu–BTC. Herein, three transition metals, namely, Zn 2+ , Ni 2+ and Co 2+ , were assessed to fabricate M−Cu−BTC, a desirable isoreticular bimetal. Results demonstrated the feasibility of using Zn 2+ to fabricate an isoreticular bimetallic Zn–Cu–BTC. The Zn 2+ doping content of Zn–Cu–BTC was varied to investigate its influence on the hydrogen sulfide (H 2 S) and methyl sulfide (CH 3 SCH 3 ) removal performance of Cu–BTC. The experimental results indicated that the sulfides removal performance of Zn–Cu–BTC increased and then decreased with increasing Zn doping content. The highest H 2 S and CH 3 SCH 3 removal capacities of 84.3 and 93.9 mg S/g, respectively, were obtained when the Zn 2+ doping content was 17%. The hybridisation of Zn and Cu in Zn–Cu–BTC induced a strong interaction between them. This interaction increased the binding energies of H 2 S and CH 3 SCH 3 towards the Cu and Zn adsorption sites while weakening the bond order between Zn and Cu. The weakened bond order made the Zn–Cu bonds easier to form metal sulfides during desulfurization process, thereby synergistically enhancing sulphide removal.
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Nano Research
·
2023
·Vol. 16
·期 5
·6670-6678
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IF 9.9
Jing Tianyun,Yang Shaokang,Feng Yonghai,Li Tingting,Zuo Yunpeng,Rao Dewei
Co-based catalysts are promising alternatives to precious metals for the selective and effective oxidation of 5-hydroxymethylfurfural (HMF) to the higher value-added 2,5-furandicarboxylic acid (FDCA). However, these catalysts still suffer from unsatisfactory activity and poor selectivity. A series of N-doped carbon-supported Co-based dual-metal nanoparticles (NPs) have been designed, among which the Co-Cu 1.4 -CN x exhibits enhanced HMF oxidative activity, achieving FDCA formation rates 4 times higher than that of pristine Co-CN x , with 100% FDCA selectivity. Density functional theory (DFT) calculations evidenced that the increased electron density on Co sites induced by Cu can mediate the positive electronegativity offset to downshift the d-band center of Co-Cu 1.4 -CN x , thus reducing the energy barriers for the conversion of HMF to FDCA. Such findings will support the development of superior non-precious metal catalysts for HMF oxidation.
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RSC Advances
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2023
·Vol. 13
·期 13
·8915-8922
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IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Le He,Gang Ding,Sasha You,Si Lu,Xianfeng Huang,Ling Li,Xiaolan Yu
Nanozymes that mimic the catalytic reaction of natural enzymes show great prospects for tumor catalytic therapy because they possess the properties of nanomaterials and natural enzymes. However, the therapeutic effect of nanozymes is restricted by the low catalytic efficiency and specific oxidation–reduction systems in the tumor microenvironment (TME), such as overexpressed glutathione (GSH) level. In order to improve the catalytic efficiency, a multifunctional nanozyme, Cu/zeolitic imidazolate framework-67 (ZIF-67)/Prussian blue (PB), was designed through the modification of Prussian blue (PB) on the surface of the copper-doped zeolitic imidazolate framework, which can be used for imaging-guided synergistic therapy with photothermal-enhanced multienzyme-like catalytic therapy and chemotherapy. The doping of Cu2+ provided better glutathione oxidase-like (GPx-like) activity and peroxidase-like (POD-like) activity to deplete GSH and increase the generation of •OH in TME. The modification of PB provided better catalase-like activity (CAT-like) to promote the production of O2 and enhance the multienzyme-like catalytic therapy. In vivo experiments showed a satisfactory anticancer effect. This work thus provided a strategy for designing a type of multifunctional nanozyme for imaging-guided combination therapy.
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