Nano Research
·
2023
·Vol. 16
·期 7
·9116-9124
·
IF 9.9
Si Lianxi,Li Hui,Zhang Yu,Zhang Donghao,An Xiaowei,Yao Mengmeng,Shao Yuanyuan,Zhu Jesse,Hu Shi
Ultrathin Pd nanosheets (NSs) have great advantages in catalysis due to their large specific surface area and high percentage of under-coordinated atoms. However, the electrochemical performance still can be improved via composition-controllable growth of their solid solution. Herein, seeded alloying strategy was proposed to synthesize Pd-Cu solid solution from Pd NSs and Pd-Cu nanostructures with tunable molar ratios obtained by changing the amount of Cu precursor. As compared to the pristine Pd NSs, the Pd-Cu solid solution shows significantly enhanced methanol oxidation reaction (MOR) performance over those of Pd NSs and homemade Pd/C as the incorporation of Cu weakens the adsorption of CO intermediate on Pd in the MOR process. The choice of template is pivotal to the growth, as a shape-dependent behavior could be identified in the alloying of Cu with Pd nanosheets enclosed by {111} and {100} facets, Pd nanocubes enclosed by {100} facet, and Pd nano-tetrahedrons enclosed by {111} facet. The Pd-Cu solid solution with tunable composition can only be obtained from Pd NSs and the shape-dependent alloying process is mainly determined by the diffusion barrier and the minimum diffusion depth of the different facets.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Shi-Xian Guan,Tao Xu,Jian-Yong Zhang,You-Guo Luo,Xingwu Zhai,Na Zhang,Yong-Zheng Fang,Qin-Fei Ke
Herein, we developed a multimodal antibacterial nanoplatform via synergism effect including knife-effect, photothermal, photocatalytic induced reactive oxygen species (ROS), and Cu 2+ inherent attribute. Typically, 0.8-TC/Cu-NS possesses higher photothermal property with the higher photothermal conversion efficiency of 24% and the moderate temperature up to 97 °C. Meanwhile, 0.8-TC/Cu-NS exhibits the more active ROS, 1 O 2 and ·O 2 - . Hence, 0.8-TC/Cu-NS possesses best antibacterial properties against S. aureus and E. coli in vitro with efficiency of 99.94%/99.97% under near-infrared (NIR) light, respectively. In the therapeutic practical use for wound healing of Kunming mice, this system exhibits outstanding curing capacity and good biocompatibility. Based on the electron configuration measurement and density functional theory (DFT) simulation, it is confirmed that the electrons on CB of Cu-TCPP flow fleetingly to MXene trough the interface, with redistribution of charge and band upward bending over Cu-TCPP. As a result, the self-assembled 2D/2D interfacial Schottky junction have made great favor to accelerate photogenerated charges mobility, hamper charge recombination, and increases the photothermal/photocatalytic activity. This work gives us a hint to mostly design the multimodal synergistic nanoplatform under NIR light in biological applications without drug resistance.
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Journal of Water Process Engineering
·
2023
·
IF 7
Xinrui Liu,Rui Guo,Xia Qin,Cuicui Xu
In this work, a Ni foam/CNTs/Cu composite electrode was prepared via the impregnation and electrodeposition methods. The electrode enhanced the total nitrogen removal and N 2 selectivity , when served as a cathode for NO 3 − -N reduction. SEM, EDS, XRD, and XPS characterization revealed that both CNTs and metallic copper were introduced onto the surface of the Ni foam substrate successfully. Besides, the LSV, CV, EIS and C dl results indicated more electrochemical active sites were in the Ni foam/CNTs/Cu electrodes than in Ni foam/Cu electrodes. Under optimal preparation conditions, the Ni foam/CNTs/Cu electrode showed N 2 selectivity of 68.89 % and nitrate removal rate of 96.75 % in 100 mg/L nitrate solution with Na 2 SO 4 as electrolyte. The selectivity of N 2 could be significantly enhanced by adding Cl − as electrolyte, and the nitrogen selectivity increased with the increase of Cl − concentration. At 1.25 g/L NaCl, the Ni foam/CNTs/Cu electrode could achieve >95 % nitrate and total nitrogen removal and close to 100 % N 2 selectivity. The N 2 selectivity of the Ni foam/CNTs/Cu electrode was 2.534 and 1.8 times of the Ni foam/Cu electrode when 0.5 g/L Na 2 SO 4 and 0.5 g/L NaCl were used as electrolytes, respectively. Consequently, to achieve the same nitrate reduction effect, the Ni foam/CNTs/Cu electrode could reduce the amount of NaCl compared with Ni foam/Cu electrode. The electrodes were tested in 6 cycles and proved to be stable. At last, a potential mechanism of nitrate‑nitrogen removal by the electrocatalytic process was suggested.
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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2023
·Vol. 43
·期 6
·1963-1978
·
IF 3.6
Lv Huan,Liu Xinyuan,Hao Yingzi,Yi Yanhui
The industrial utilization of methane to methanol is based on the indirect pathway with syngas as an intermediate product, but the reaction conditions are very harsh and the costs in equipment and operations are extremely high. Therefore, the direct oxidation of methane to methanol (DOMTM) under mild conditions is more desirable. In this paper, coupling of non-thermal plasma and Cu–zeolite (Cu–ZSM-5 and Cu–S-1) catalysts have been studied for DOMTM. The effect of Si/Al ratios (Cu–ZSM-5 and Cu–S-1 catalysts) on the reaction performance has been investigated. Cu–S-1 catalyst exhibited the best catalytic performance, i.e., 5.8% methane conversion and 50.6% methanol selectivity. The employed catalysts have been characterized by XRD, UV–Vis, XPS and FT-IR. The results show that Cu–ZSM-5 catalysts with high Si/Al ratio are conducive to the formation of isolated Cu 2+ species, and Cu–S-1 catalyst exhibits the most abundant isolated Cu 2+ species. Furthermore, Cu–S-1 catalyst shows the most abundant O ads species. The plentiful surface silicon defects on S-1 is the reason why Cu–S-1 catalyst shows the most abundant isolated Cu 2+ and O ads species, and these two species are interdependent to form a Si–O–Cu species, which may be the active site for DOMTM. Based on these findings, the possible catalytic mechanism was proposed.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Yankai Liu,Ruinian Zhou,Jianyu Qu,Feng Han,Shuai Zhang,Xingliang Xu
Upgrading carbon dioxide (CO 2 ) into valuable products is a highly promising strategy of artificial carbon cycle. In this study, a series of in situ reduced CuMgAl layered double hydroxides (R-CuMgAl-LDHs) composites were synthesized, in which Cu nanoparticles were effectively dispersed and anchored on MgAl-LDHs with formation of Cu + and Cu 0 species. The optimized R-Cu 1.5 Mg 1.5 Al 1 -LDH exhibited excellent catalytic performance for the carboxylative cyclization of 2-methyl-3-butyn-2-ol with CO 2 (turnover number of 243) under mild conditions. The layered structure of LDH stabilized the active Cu species with high dispersion, enhancing the catalytic efficiency of this carboxylative cyclization reaction. Simultaneously, the dual-activation of both CO 2 and propargylic alcohol by Cu 0 /Cu + species generated on the surface of LDH contributed significantly to the catalytic efficiency enhancement. Furthermore, R-Cu 1.5 Mg 1.5 Al 1 -LDH catalyzed the reaction of a wide range of terminal or internal propargyl alcohols with CO 2 , yielding various functionalized α-alkylene cyclic carbonates. Finally, a reasonable reaction mechanism was put forward according to the comprehensive analysis.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Bingqiao Yang,Pengliang Huang,Qing An
A small molecular triazole derivative called AMT (3-amino-5-mercapto-1,2,4-triazole) was explored as a novel and efficient chalcopyrite depressant in the preferential flotation of chalcopyrite from molybdenite. The flotation performances were comprehensively investigated via micro-flotation tests of singe and mixed minerals with and without Cu collector. The adsorption mechanisms were determined in terms of contact angle, adsorption capacity, and zeta potential, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and DFT calculations. Single mineral flotation results illustrated that the AMT selectively depressed chalcopyrite over a wide range of pH values. Particularly, AMT was able to depress chalcopyrite even in the presence of sodium isobutyl xanthate (SIBX). The contact angle, adsorption capacity, zeta potential, and FTIR results suggested that AMT was preferentially adsorbed on chalcopyrite surface, but it barely interacted with molybdenite. XPS tests and DFT calculations demonstrated that AMT was chemically adsorbed on chalcopyrite surface through the hybridization of S (1) and N (1) 2p orbitals of AMT with the Cu (1) 3d orbital. The bonding between S (1) atom and Cu (1) was much stronger than that between N (1) and Cu (1). Thus, AMT exhibited good potential as a novel depressant due to its excellent selectivity and practicability.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Fuad Abduro Bushira,Shimeles Addisu Kitte,Yong Wang,Haijuan Li,Ping Wang,Yongdong Jin
In this study, an effective oxygen vacancy (Ov)-involved luminol-dissolved oxygen (O2) electrochemiluminescence (luminol-DO ECL) system was developed and exploited for ECL sensing applications through significant plasmon enhancement of the Ov-involved weak luminol-DO ECL signals by the combined use of Cu-doped TiO2 oxygen vacancy and a Au@SiO2 nanomembrane. The results disclosed that the ECL response of the corresponding system could be synergistically boosted, and the plausible underlying mechanism has been discussed. Furthermore, for the first time, the developed system has been successfully applied for the highly sensitive detection of alkaline phosphatase with a low limit of detection of 0.005 U/L, with an excellent linear range from 0.005 to 10 U/L, as well as good stability and reproducibility.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Yue Ma,Songqi Cheng,Xiaodong Wu,Tongxi Ma,Liping Liu,Baofang Jin,Minghan Liu,Jianbo Liu,Rui Ran,Zhichun Si,Duan Weng
To improve the hydrothermal durability of Cu-SSZ-13 selective catalytic reduction (SCR) catalyst, a thin Al 2 O 3 modification layer was coated on the external surface of Cu-SSZ-13 by a chemical liquid deposition (CLD) method. The high-temperature SCR activity of the Al-modified Cu-SSZ-13 can be maintained upon 750–800 °C hydrothermal aging, and over-oxidation of NH 3 is largely inhibited. Based on H 2 -TPR and EPR results, it is revealed that CuAl 2 O 4 -like species forms upon Al modification and converts further to CuAlO 2 -like species during aging, while the accumulation of CuO-like species is inhibited. The high affinity of Al-containing species ( i.e. , Al 2 O 3 and CuAl 2 O 4 -like species) with Cu(OH) 2 is suggested by DFT calculations, indicating that Cu(OH) 2 detached from ion-exchange sites are captured by Al to form CuAlO 2 -like species instead of CuO-like species. The passivation of detached Cu species by coated Al leads to somewhat weakened low-temperature SCR activity, but successfully preserves the high-temperature SCR performance upon aging, which can be applied to high-temperature SCR scenarios.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Liu,Taixin Liang,Jiangbo Zhang,Fei Xiao,Houhe Chen
Intermolecular energetic materials (IEMs) have become the focus of attention due to their excellent performance in combustion, ignition, energy release and sensitivity. In this paper, two IEMs were successfully designed and prepared by the self-assembly of 5-aminotetrazole (5-ATZ) and transition metal ions on the surface of ammonium perchlorate (AP) particles. The scanning electron microscope, infrared spectroscopy, powder X-ray diffraction, thermogravimetric analyses, and differential thermal analyses were employed to characterize the prepared samples. The results show that the surface of AP particles is completely covered by a uniform and dense M(5-ATZ) 4 Cl 2 (M = Cu, Co) self-assembled layer. Thermal analyses show that the high-temperature decomposition peak temperatures of AP/Cu(5-ATZ) 4 Cl 2 (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 (10 wt%) are decreased by 93.3 °C and 127.1 °C compared to the case of pure AP, while the heat releases of them are increased by 539 J∙g −1 and 580 J∙g −1 . In addition, the burning rates of AP/Cu(5-ATZ) 4 Cl 2 /Al (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 /Al (10 wt%) are increased by 6.8 mm∙s −1 and 7.8 mm∙s −1 compared with the case of AP/Al. Moreover, the hygroscopicity tests show that the prepared samples do not agglomerate aftter being placed in the atmosphere with a relative humidity of 79% for 66 h. This research shows considerable application prospects in improving the combustion and energy performance of solid propellants, it is also a reference for the design and preparation of other novel IEMs.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Zhang Li,Yang Xiaoju,Yuan Qing,Wei Zhiming,Ding Jie,Chu Tianshu,Rong Chao,Zhang Qiao,Ye Zhenkun,Xuan Fu-Zhen,Zhai Yueming,Zhang Bowei,Yang Xuan
Understanding the structure-stability relationship of catalysts is imperative for the development of high-performance electrocatalytic devices. Herein, we utilize operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to quantitatively monitor the evolution of Cu single-atom catalysts (SACs) during the electrochemical reduction of CO 2 (CO 2 RR). Cu SACs are converted into 2-nm Cu nanoparticles through a reconstruction process during CO 2 RR. The evolution rate of Cu SACs is highly dependent on the substrates of the catalysts due to the coordination difference. Density functional theory calculations demonstrate that the stability of Cu SACs is highly dependent on their formation energy, which can be manipulated by controlling the affinity between Cu sites and substrates. This work highlights the use of operando ATR-SEIRAS to achieve mechanistic understanding of structure-stability relationship for long-term applications.
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RSC Advances
·
2017
·Vol. 7
·期 80
·51001-51007
·
IF 3.108
Chun-Nan Zhu,Dong-Yun Zheng,Hui-Min Cao,Shan-Ying Zhu,Xiao-Jun Liu
Ternary I–III–VI nanocrystals (NCs) without toxic elements, such as Cu–In–S, are promising candidates for biolabeling and bioimaging due to their favorable biocompatibility. At present, it remains a tremendous challenge to directly synthesize high-quality Cu–In–S/ZnS core/shell NCs in aqueous solution at atmospheric pressure. Herein, a simple and reliable strategy that combines the hot-injection method and successive ion layer adsorption and reaction has been proposed to realize aqueous synthesis of fluorescent Cu–In–S/ZnS core/shell NCs. The growth of ZnS shell around Cu–In–S NCs not only improved the fluorescence quantum yield by several hundred times and to the value of 18%, but also effectively enhanced their fluorescence stability by protecting Cu+ in Cu–In–S core from being oxidized to Cu2+. The prepared Cu–In–S/ZnS core/shell NCs with bright and stable fluorescence were conjugated with wheat germ agglutinin and further applied to cancer cell imaging. This strategy here should open new avenues for aqueous synthesis of high-quality nanomaterials with the core/shell structure for broad biomedical applications.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2026
·
IF 3.6
Cheng Song,Tinghui Liu,Xiaohui Yang,Xingzu Wang,Hong Liu
Electrocatalytic nitrate (NO 3 − ) reduction offers a sustainable route for simultaneous NO 3 − remediation and ammonia (NH 3 ) production, yet its efficiency is limited by the competing hydrogen evolution reaction (HER) and the imbalance between NO 3 − activation and hydrogen supply. Herein, Co–Cu bimetallic sulfide nanoflowers were synthesized via a one-step hydrothermal method and optimized for NO 3 − to NH 3 conversion. The Co 0.9 Cu 0.1 S nanoflowers, assembled from two-dimensional nanosheets, delivered 97.83% ± 1.71% nitrate conversion, nearly complete NH 4 + -N selectivity, and a Faradaic efficiency of 98.52% ± 0.83% at −0.75 V vs. RHE. Systematic Co/Cu-ratio studies, electrochemical kinetics, Bode analysis, hydrogen adsorption/desorption behavior, and XPS results reveal that Cu promotes NO 3 − activation and electronically modulates Co sites, while Co facilitates reactive hydrogen generation and utilization. This synergy enables on-demand hydrogen supply, directing hydrogen toward NO 3 − hydrogenation rather than HER. pH-dependent tests further identify a neutral electrolyte as favorable for balancing proton supply and competitive HER. Graphical Co–Cu bimetallic sulfide nanoflowers enable efficient nitrate-to-ammonia conversion through on-demand hydrogen supply. Cu sites promote nitrate activation, while Co sites regulate reactive hydrogen generation and consumption, thereby enhancing ammonia selectivity and suppressing competitive hydrogen evolution.
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