MICROPOROUS AND MESOPOROUS MATERIALS
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2023
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IF 5.2
Congli Li,Jiang Wang,Zhenfei Wang,Jinxiang Dong,Qi Shi
CuCl/NaY is the most representative π-complexation adsorbent, prepared by solid thermal dispersion followed by vacuum thermal activation. However, determining the autoreduction behavior of Cu species for CuCl/NaY adsorbent in vacuum thermal activation has rarely been researched. This study characterized the valence state, location, and types of Cu species during thermal dispersion and vacuum activation. During the thermal dispersion, Cu species were uniformly dispersed into NaY micropores. Under vacuum activation at 100 °C, the location of Cu species changed, migrating from supercages to near the plane (toward the sod cage or the supercage side) of the 6-membered ring connecting the supercage and sod cage. However, by activating at 150 °C, vacuum autoreduction occurred: (Cu 2+ –O − )Cl − species evolved into Cu + Cl − species. This was accompanied by the migration of Cu(I) species to the appropriate CO adsorption site on the plane center of the six-membered ring connecting the supercage and sod cage in the NaY framework, which achieved confined dispersion. The CO adsorption capacity of CuCl/NaY activated at 150 °C was 2.75 mmol/g, significantly higher than when activated at 100 °C. When activated at 200 °C, Cu(II) species was further reduced to Cu(I) slightly, which had not migrated to an effective adsorption site. Our results show the Cu species’ evolution and autoreduction behavior for CuCl/NaY adsorbent under vacuum thermal activation, and they can serve as a reference to guide the preparation of π-complex adsorbents.
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JOURNAL OF NANOPARTICLE RESEARCH
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2023
·Vol. 25
·期 11
·1-12
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IF 2.5
Li Fangyuan,Yao Niu,Yuan Huiyu,Cui Junyan,Jia Quanli
The redox properties of electrode materials play a vital role in electrochemical performance. Fabrication of electrode materials with multiple oxidation species is highly desired for ultrasensitive glucose sensing. Herein, multivalent Cu/Cu 2 O/CuO/C (Cu/C) nanocomposites were successfully prepared for non-enzymatic glucose sensing by in situ pyrolysis of Cu metal-organic framework (Cu 3 (BTC) 2 ·3H 2 O, Cu-BTC) at a critical temperature. Structure characterizations showed that the nanocomposites maintained the original morphology of Cu-BTC crystals and exhibited mesoporous structures. Meanwhile, multiple Cu species containing Cu, Cu 2 O and CuO were generated simultaneously, which were tightly pinned on the ligand-derived carbon layers. Thus, under the synergistic effect of multivalent Cu species, mesoporous structure and intense interface contact, the sensing platforms based on Cu/C nanocomposites exhibited good glucose detection performance with a wide linear range of 0.005-2.0 mM, ultrasensitivity of 147.65 μA mM -1 cm -2 , low detection limit of 6.31 μM (S/N = 3), and favorable anti-interference properties and stability. Especially, the Cu/C sensing platform showed excellent recoveries of glucose when used to monitor glucose in real sample of honey. The good electrochemical activities of Cu/C nanocomposites render them promising candidates for sensors and other applications. Graphical abstract
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Acta Biomaterialia
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2023
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IF 9.7
Xu Jin,Jie Shan,Jiemin Zhao,Tao Wang,Wei Zhang,Shijie Yang,Haisheng Qian,Liang Cheng,Xu-Lin Chen,Xianwen Wang
Infections and oxidative stress complicate wound healing. In recent years, nanomaterials with natural enzymatic activities have enabled the development of new antibacterial pathways. In this study, Cu-Fe 3 O 4 nanoclusters with multienzyme properties were synthesised. Interestingly, they exhibited activity similar to that of horseradish peroxidase (POD) in acidic environments but their functions resembled superoxide dismutase and catalase in neutral or weakly alkaline environments. In vitro studies have demonstrated the good free-radical scavenging activity of Cu-Fe 3 O 4 nanoclusters in a neutral environment. Under acidic conditions, Cu-Fe 3 O 4 nanoclusters combined with H 2 O 2 demonstrated good antibacterial activity against methicillin-resistant Staphylococcus aureus ( MRSA ) and Escherichia coli ( E. coli ). The combination of Cu-Fe 3 O 4 and H 2 O 2 was found to be effective in preventing MRSA infections and promoting wound healing in animal models. RNA sequencing (RNA-seq) technology revealed that chemodynamic therapy (CDT) using nanoparticles can interfere with metabolic processes such as galactose metabolism in MRSA bacteria, destroy the transport system on the surface of MRSA , and affect quorum sensing to hinder the formation of biofilms, thus achieving effective antibacterial efficacy. The use of Cu-Fe 3 O 4 nanoclusters as a novel class of multi-catalytically active nanozymes in the anti-infection of disease-causing pathogens and wound healing has significant potential. Statement of Significance Cu-Fe 3 O 4 nanoclusters with multienzyme properties were successfully prepared by a solvothermal method. Cu-Fe 3 O 4 nanoclusters exhibited horseradish peroxidase (POD)-like activity in acidic environments and also showed synergistic effects similar to superoxide dismutase peroxidase in neutral or weakly basic environments. More importantly, these Cu-Fe 3 O 4 nanoclusters showed high biosafety with no apparent in vivo toxicity. Chemodynamic therapy (CDT) using Cu-Fe 3 O 4 nanoclusters was revealed by RNA sequencing (RNA-Seq) technology to interfere with the metabolic processes of MRSA bacteria, such as galactose metabolism, disrupt the MRSA surface transport system, and impede biofilm formation, resulting in effective antibacterial efficacy. The use of Cu-Fe 3 O 4 nanoclusters for anti-infection and wound healing of pathogenic pathogens has significant potential as a novel class of multi-catalytic active nanoclusters.
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FUEL
·
2023
·
IF 7.4
Jing Li,Tingshan Chan,Chuanyong Jing,Jin Wang
Selective conversion of CO 2 to fuels and chemicals has been considered one of the key challenges in the photocatalytic CO 2 reduction reaction. The multi-electron reduction reaction requires the design of photocatalysts that can adsorb CO 2 and transfer electrons. Herein, Cu single atoms are confined in a conjugated microporous polymer (CMP) to construct Cu n @CMP photocatalyst for CO 2 reduction to produce C 2 H 4 and CH 4 . By adjusting Cu loading, Cu 0.012 @CMP exhibited a high performance with production yields of 236.81 μmol·g −1 ·h −1 for C 2 H 4 , and 78.2 % selectivity for C 2 H 4 formation. DFT calculations displayed the band structure and confirmed Cu–N together with characterization. The in situ DRIFTS revealed *CH 2 and *C 2 H 4 as key reaction intermediates to form CH 4 and C 2 H 4 , respectively. The synergy effect in Cu single-atoms and CMP contributed greatly to C–C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO 2 to C 1 /C 2 . This work highlights the potential for constructing Cu single atoms on CMP to produce highly selective C 2 H 4 .
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INORGANIC CHEMISTRY COMMUNICATIONS
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2023
·
IF 3.8
Miaomiao Li,Ying Li,Chunping Li,Tong Xu,Yinghui Sun,Jie Bai
Herein, the composite catalyst supported by Pd-Cu bimetal was prepared by hydrothermal synthesis method using carbon nanofibers anchored LZ-276 zeolite as carrier. The addition of Cu not only save cost but also realize the high dispersion of metal nanoparticles. Under the optimized reaction conditions, the catalyst exhibits excellent catalytic activity and cycle stability in the Suzuki-Miyaura reaction. The designed structure effectively improves the catalytic performance of metal nanoparticles catalyzed reaction, and would inhibit the leaching or aggregation of metal particles. The strategy of reducing the noble metals dosage by using non-noble metals to replace noble metals reduces the catalyst costs, and thus holding great promise for industrial application.
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Nano Energy
·
2023
·
IF 17.6
Hao Zhang,Ying Wang.,Qiong Lei,Ying Wang,Chiu Tang,Jun Yin,Tsz Woon Benedict Lo
Tracking the evolution of electrocatalysts over oxide-derived Cu materials during the electrochemical CO 2 reduction reaction (eCO 2 RR) is pivotal for optimizing the product selectivity toward desired multi-carbon (C 2+ ) products. However, the identification of the true intermediate active catalyst is still unclear. Here, we adopted a multi-modal characterization approach, primarily based on operando powder X-ray diffraction and operando micro-Raman spectroscopy, to study three Cu 2 O precursors with different morphologies, namely, octahedral (O-), cubic (C-), and nanowire (N-Cu 2 O). This multi-modal approach allows us to investigate the Cu 2 O nano-crystallites from the interface to the bulk structure. The results suggested notably different electrochemical reduction kinetics. 26.1% O-Cu 2 O and 90.6% C-Cu 2 O were reduced to much smaller Cu(0) domains after two hours of time-on-stream; N-Cu 2 O, with notably higher surface-to-volume ratio, was completely reduced within 45 min of time-on-stream. We accordingly observed a structure-reactivity correlation where a more intricate Cu 2 O/Cu grain network (and hence Cu + -Cu 0 junctions) as observed in O-Cu 2 O, can lead to stable and quantitative production of ethylene at the Faradic efficiency of around 40% (in stark contrast to those of C- and N-Cu 2 O). The synergy between the Cu 2 O and Cu phases was also verified by density functional theory calculations. The upshifted d -band center of Cu 2 O/Cu in O-Cu 2 O is the most conducive toward the production of ethylene, whereas the downshifted d -band center of Cu 2 O/Cu in C-Cu 2 O leads to a decreased production of ethylene in the expense of unwanted production of hydrogen. We envisage that system optimization and design of new catalysts will become more facile and efficient using a related multi-modal operando characterization philosophy.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Zuan Yu,Jiangwei Xie,Tianlun Ren,Hongjie Yu,Kai Deng,Ziqiang Wang,Hongjing Wang,Liang Wang,You Xu
Utilizing nitrate from wastewater as a N-source for ammonia synthesis via electrocatalysis is of significance for both environmental protection and ecological nitrogen cycle balance, which requires high-performance electrocatalysts to drive selective nitrate-to-ammonia transformation. In this work, an electrochemical postmodification strategy was developed to regulate the surface structure of presynthesized Cu nanodendrites at the atomic level. A combination of physicochemical characterization and electrochemical study demonstrates that such a treatment could induce surface Cu atom rearrangement and result in increased electrochemically active surface area and high density of surface-active sites, disclosing a high electrocatalytic nitrate-to-ammonia capability, with an optimal NH3 yield rate of 0.2238 mmol h–1 cm–2 and a corresponding Faradaic efficiency of 94.43%. This study may provide a guiding design avenue for atomic arrangement engineering of metallic nanocrystals via electrochemical postmodification for nitrate reduction reaction and other energy conversion electrocatalysis.
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DALTON TRANSACTIONS
·
2023
·
IF 4
Ruifeng Wang,Qiyuan Pan,Fang Li,Jingying Guo,Yaru Huo,Chao Xu,Manwen Xiong,Ziyong Cheng,Min Liu,Jun Lin
Caries as a result of acid demineralization is the most common oral microbial infection disease. Due to the small and complex intraoral operating space, it is challenging to completely remove Streptococcus mutans (S. mutans) and other cariogenic bacteria. As an intelligent acid-responsive photosensitive nanomaterial, O2-Cu/ZIF-8@Ce6/ZIF-8@HA (OCZCH) was chosen to adapt the anaerobic and acidic microenvironment to inactivate S. mutans. In this work, OCZCH not only has a regular nanomorphology under the SEM and TEM images but also has an intelligent acid responsiveness as evidenced by the release of Ce6 and oxygen. When excited by near-infrared light at 650 nm, Ce6 released reactive oxygen species (ROS) that act synergistically with internal oxygen to significantly enhance the antimicrobial therapeutic effect of photodynamic therapy (PDT). In vitro, antimicrobial experiments showed that OCZCH could achieve an impressive sterilization effect against S. mutans and the biofilm. Notably, the acid-producing ability of the bacteria was also significantly inhibited. Considering its oxygen-carrying photosensitizing properties, excellent responsiveness to acidic environments, and antimicrobial capacity under anaerobic conditions, OCZCH is considered an innovative candidate for clinical application in treating dental caries.
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Journal of Water Process Engineering
·
2023
·
IF 7
Qingsheng Xu,Zhengbo Yue,Rui Deng,Xinquan Wang,Xiao He,Xin Chuai,Shaoping Wang,Jin Wang
The alkaline sludge produced by the neutralization treatment of acid mine drainage (AMD) is not only large and difficult to treat, but also prone to secondary pollution. The cost of conventional sludge treatment technology is high, so there is an urgent need to develop new methods. The process of neutralizing AMD is similar to the co-precipitation reaction of LDHs, so the cost of recovering LDHs from AMD is lower, but the application performance of LDHs is limited by the stacking of laminates. In this paper, the structure of LDHs was optimized by adding biochar (BC) during the neutralization process of AMD. After adding 40 % BC, the crystal planes of alkaline sludge based LDHs (AS-LDHs) became more parallel, and the adsorption properties of Cd and Cu were increased by 2.7 and 1.95 times, with the maximum adsorption amounts of 901.5 and 231.3 mg/g, respectively. The relevant removal mechanism was investigated in depth at the electronic scale by experiments combined with DFT calculations. Since AS-LDHs have the advantages of good acid stability, low zero-point charge and strong adsorption and regeneration capacity, this method has a broad application prospect.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Yunjiang Yu,Zheng Huang,Dongyang Deng,Yongming Ju,Luyao Ren,Mingdeng Xiang,Liangzhong Li,Hui Li
Tetrabromobisphenol A (TBBPA) was a potential persistent organic pollutants. This study synthesized s-Fe/Cu bimetallic particles by decorated sponge iron (s-Fe) with Copper (Cu) to degrade TBBPA. S-Fe/Cu bimetallic particles was further characterized by XRD, XPS, SEM and EDS. The optimal TBBPA removal efficiency was 95.9%. Among the theoretical Cu mass loading increasing from 0 wt% to 6 wt%, 4 wt% mass loading was the best; with TBBPA initial concentration increased from 5 mg/L to 30 mg/L, TBBPA removal efficiency decreased from 91.2% to 73.0%; also, when dosage increased from 10 g/L to 30 g/L, removal efficiency increased from 58.1% to 95.9%; pH 6.5 were beneficial to degrading TBBPA and the s-Fe/Cu bimetallic particles showed strong catalytic ability after 4 reuse cycle. Kinetic analysis showed that the degradation of TBBPA obeyed pseudo-first-order kinetics. In addition, Liquid Chromatography Time-of-Flight Mass Spectrometry (LC/TOF/MS) detected degradation products including debromination products, hydroxylation products, single aromatic ring products and O -methylating product, which demonstrated that the main degradation pathway were debromination, hydroxyl, β -scission and O -methylation reactions.
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FUEL
·
2023
·
IF 7.4
Yang Shen,Chunjiang Liu,Cunhao Cui,Hairong Ren,Mingming Gu,Haoran Liu,Zhongyue Zhou,Fei Qi
Lignin catalytic pyrolysis presents a promising and sustainable approach to producing aromatic molecules. Herein, we investigated the effect of modified zeolite with copper (Cu/HZSM-5) catalyst on efficiently pyrolyzed kraft lignin into aromatic hydrocarbons (AHs) production, especially mononuclear aromatic hydrocarbons (MAHs). Time-of-flight mass spectrometry (TOF-MS) was employed to compare the volatile product profiles of lignin during catalytic pyrolysis. The highest yield of MAHs reached 70.59 mg/g based on dry lignin at 550 °C, accounting for 70.23% among lignin pyrolysis products, compared to the pristine HZSM-5 zeolite catalytic system with MAHs yield of only 54.31 mg/g and of 40.34% in products. At 550 °C and 60 s residence time, the 5% Cu/HZSM-5 catalyst demonstrated the best performance compared to all other catalysts in terms of selectively producing MAHs. The results are ascribed to the enhancement of decarboxylation and aromatization processes by the doping of copper. This work demonstrates a cost-effective pathway that potentially converts kraft lignin into aromatic hydrocarbon production at a phenomenally high selectivity, providing a concept for industrial application toward biomass utilization and high value-added production.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
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