DALTON TRANSACTIONS
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2023
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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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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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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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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
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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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INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
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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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 28
·期 29
·39513-39523
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IF 4.223
He Jun,Song Wenchao,Huang Xiaohan,Gao Zuoyu
Magnesium oxide/expanded graphite (MgO/EG) catalyst was synthesized and applied for enhancing the degradation of Cu-ethylenediaminetetraacetic acid (Cu-EDTA) in an aqueous solution. The MgO/EG catalyst was characterized by XRD, SEM, EDS, and FTIR. For assessing the catalytic activity of MgO/EG, essential influencing factors were investigated including catalyst dosage, O 3 dosage, initial pH, initial Cu-EDTA concentration, and coexisting ions. The results show that the catalytic material showed high catalytic oxidation capacity for the Cu-EDTA removal in the MgO/EG/O 3 system. 100% of Cu(II) and 73.2% of TOC removal efficiency could be achieved in the MgO/EG/O 3 system at the reaction times of 90 min. This efficiency was higher than that seen for other systems, including O 3 alone (Cu(II) 81.4%/TOC 60.6%), EG/O 3 (84.2%/64.1), MgO/EG (< 4%/< 4%), and EG (< 4%/< 4%). A small decrease in the Cu(II) and TOC removal rate was observed after three runs in the stability and reusability experiments of the catalyst. Assays with radical scavenging experiments confirmed that MgO/EG-mediated oxidation was dependent on a hydroxyl radical pathway. The UV–vis spectra confirmed that the absorption peak of Cu-EDTA was gradually decreased and finally disappeared.
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Surfaces and Interfaces
·
2021
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IF 4.837
Zepeng Fang,Dagui Chen,Fengpo Yan,Jiangquan Lv,Yongjing Wang,Xiangfeng Guan
The water monitoring parameter of chemical oxygen demand (COD) is a universal way to assess organic pollution in aqueous systems. Though the ways for the detection of COD have been developed for decades, it is still a challenge to achieve highly sensitive and portable COD detectors. In this work, a new electrode composite of Ni/ZnO/Cu (CE-1) was prepared for the electrochemical tests of COD. The electrode was structural characterized by using scanning electron microscope (SEM), transmission electron microscope (TEM), and X-ray Diffractometer (XRD), which showed that self-supported Cu microflowers were successfully electrodeposited on the ZnO micro-prims that were firstly loaded on the Ni foils. The electrochemical behaviors were investigated with the comparison of CE-1 and the electrode that Cu nanoparticles were directly deposited on the Ni foil (CE-2). It shows that CE-1 possesses much superior electrochemical properties than CE-2, which indicates that the introduction of ZnO micro-rod the electrode can significantly enhance the electrocatalysis property. CE-1 exhibited a linear COD detection range of 2.3603 to 577.8 mg/L as well as an excellent correlation with the classic dichromate method (R 2 = 0.99933). Moreover, low detection limit of 0.6036 mg/L (the signal blank/slope=3) and high sensitivity of 2.403 × 10 −2 mA / (mg • L −1 ) can be simultaneously achieved by using CE-1, which is hard to attain for its counterparts reported in literature. CE-1 also shows good concordance with the classic method for real water sample detections. Consequently, the environmentally friendly CE-1 is supposed as a promising candidate for COD detection electrode.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Zhengjie Gong,Tao Ma,Feng Liang
Organic dyes and nitrophenols in the textile industry are wastewater pollutants. In order to develop an efficient nanocatalysts to remove organic pollutants in wastewater, the trimetallic Ni@Cu@Pd nanoparticles (Ni@Cu@Pd NPs) with a blackberry-like structure was successfully prepared by a seed mediated growth method for the first time. The blackberry-like structure and the presence of Ni, Cu and Pd have been confirmed through TEM, SEM, EDS and XPS characterizations. Owing to the charge interaction between metal species along with blackberry-like structure, trimetallic Ni@Cu@Pd NPs delivered a record high catalytic activity toward the reduction of rhodamine B (RhB), with an apparent rate constant of 7.20 min −1 . Ni@Cu@Pd NPs also exhibited high activity for the catalytic reduction of methylene blue (MB) and 4-nitrophenol (4-NP). Moreover, the Ni@Cu@Pd NPs catalyst showed excellent stability and reusability.
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WATER RESEARCH
·
2021
·
IF 11.236
Jingxin Yang,Yujie Luo,Xianghui Fu,Zijun Dong,Chuan Wang,Hong Liu,Chengchun Jiang
Transition metal catalyzed sulfite auto-oxidation is a promising technology used in water and wastewater treatment for the elimination of contaminants. In the literature, this process has been reported to be efficient only in the presence of oxygen. However, in this study, we unexpectedly found that the degradation of diatrizoate (DTZ) by a system based on the combination of copper ion and sulfite (Cu(II)/S(IV)) reached over 95% under anaerobic conditions , but was considerably retarded under aerobic conditions at pH 7. Furthermore, it was found that Cu(I), generated from the cleavage of the CuSO 3 complex, was the main reactive species responsible for the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions. In fact, the absence of oxygen promoted the accumulation of Cu(I). The concomitant release of the iodide ion with the degradation of DTZ indicated that the anaerobic degradation of DTZ by the Cu(II)/S(IV) system mainly proceeded through the deiodination pathway, which was also confirmed by the detection of deiodinated products. The anaerobic degradation of DTZ was favored at higher initial concentrations of Cu(II) or sulfite in this system. Since the CuSO 3 complex, the precursor of Cu(I), was formed mainly at pH 7, the highest anaerobic degradation of DTZ was achieved at pH 7. An increase in reaction temperature considerably enhanced the degradation of DTZ by the Cu(II)/S(IV) system with an apparent activation energy of 119.4 kJ/mol. The presence of chloride, bicarbonate and humic acid slightly influenced the anaerobic degradation of DTZ. The experiments with real water samples also demonstrated the effectiveness of the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Xinyue He,Tao Zhang,Qing Xue,Yalan Zhou,Hailong Wang,Nanthi S. Bolan,Rongfeng Jiang,Daniel C.W. Tsang
Heavy metals removal from aqueous phase by adsorption technique has recently attracted a considerable interest. Although various adsorbing materials have been developed, introducing more functional groups is considered as the most efficient way to promote the adsorption capacity of the selected adsorbent. However, this approach is usually limited in costly modification precursor and unguaranteed loading efficacy. In this study, waste corn straw was converted to adsorbent precursor by hydrothermal carbonization . The obtained hydrochar (HC) was chemically activated before being modified by polyethyleneimine (PEI). Multiple analysis methods including Scanning Electron Microscopy, Fourier Transform Infrared analysis, and X-ray Photoelectron Spectroscopy analysis verified the alkali activated hydrochar (alkali-HC) was more efficacy to enhance PEI grafting than acid activation . Based on this, the modified HC materials obtained a better adsorption performance. The sorption process of Cu(II) and Zn(II) on the acid-PEI-HC, alkali-PEI-HC, and pristine HC fitted the pseudo second order kinetic and Freundlich model well, and was dominated by chemisorption . Among these adsorbents, the adsorption capacity of alkali-PEI-HC to metal ions was the maximum, which was 207.6 mg/g to Zn(II) and 56.1 mg/g to Cu(II) at 298 K. Regeneration tests showed a result of no less than 60% of its removal capacity was achieved after five cycles. Therefore, alkali-PEI-HC performed as a promising composite sorbent for metal ions. In addition, the study described here has provided a new basis for the utilization of hydrochar (1.08 kWh kg −1 ) derived from agricultural resources as a promising adsorbent precursor.
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CHEMOSPHERE
·
2021
·
IF 7.086
Fuyou Du,Zhan Lai,Huiyang Tang,Haiyan Wang,Chenxi Zhao
In this work, a novel BiOCl/Cu-doped Bi 2 S 3 photocatalyst was designed to efficiently remove ciprofloxacin (CIP) with high photocatalytical activity and good stability over a wide pH range. Compared with Cu-doped Bi 2 S 3 , Bi 2 S 3 , BiOCl, BiOCl/Bi 2 S 3 , and Cu-doped BiOCl, the photocatalytical degradation rate of CIP (97.1% at 20 mg/L) over BiOCl/Cu-doped Bi 2 S 3 was enhanced by about 84.77, 44.23, 2.95, 2.27, and 1.96 times within 20 min, respectively. Notably, the BiOCl/Cu-doped Bi 2 S 3 photocatalyst also displayed high photocatalytical performance in the degradation of other antibiotics including norfloxacin, ofloxacin, and tetracycline (40 mL, 20 mg/L; 88.3%, 100%, and 95.2% of degradation rate within 30 min, respectively) under visible light irradiation. Radical trapping experiments and electron spin resonance technique indicated that superoxide radicals (•O 2 − ) and photogenerated holes (h + ) played crucial roles in the photocatalytic degradation of CIP. Finally, the possible CIP degradation pathways was proposed by detecting the CIP intermediates in photocatalytical reaction process.
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