PLASMA CHEMISTRY AND PLASMA PROCESSING
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2023
·Vol. 43
·期 6
·1963-1978
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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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JOURNAL OF HAZARDOUS MATERIALS
·
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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Dogan Kaya,Ilker Demiroglu,Ilknur Baldan Isik,Hasan Huseyin Isik,Selda Kılıç Çetin,Cem Sevik,Ahmet Ekicibil,Faruk Karadag
Improving the activity and stability of Pt-based electrocatalysts is still crucial for hydrogen generation applications. In this study, we investigated the catalytic properties of Cu-doped Pt alloy nanostructures synthesized by the modified polyol method, and compared the performance of PtCu catalyst with that of commercially available Pt/C for the hydrogen evolution reaction (HER) at room temperature . Structural analyses revealed that the PtCu catalysts exhibited fcc- F m 3 ¯ m crystal structure with an average particle size below 5 nm. The HER performance of the catalysts showed overpotential of around −1.0 V (vs. Ag/AgCl) and Pt 0.25 Cu 0.75 and Pt 0.75 Cu 0.25 catalysts exhibited enhanced performance in 1 M KOH. The Pt 0.75 Cu 0.25 catalyst exhibited distinct performance, with the highest mass activity found to be 62.80 mA mg −1 Pt . The most active Pt 0.75 Cu 0.25 catalysis for the HER process had the lowest onset potential of 0.989 V and Tafel slope of 35.5 mV dec −1 , which were an improvement compared to commercially available Pt/C catalysts. First principle DFT calculations confirmed the stabilities of Pt 1 Cu 3 , Pt 1 Cu 1 and Pt 3 Cu 1 compositions as ordered alloy structures. Nudged elastic band method calculations and the d-band model verified the higher catalytic activity of Pt–Cu nanoparticles compared to pure nanoparticles and point out the relevance of a synergistic effect of Pt and Cu atoms on water dissociation. According to DFT calculations, Cu and Pt sites significantly influenced the adsorption of H 2 O and H, respectively, for splitting water molecules. While the Pt 59 Cu 20 cluster has the highest H 2 O adsorption energy at the (100) atop site of Cu atoms, H adsorption occurs at the (111) site of Pt atoms.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Huimin Li,Xinyuan Huang,Ye Lv,Jinli Zhang,Wei Li
The biomass electrochemical oxidation has attracted worldwide attention owning to its carbon-neutral and sustainable nature. Here, different morphologies of CoCu-carbonate hydroxides (CH) electrodes are prepared through one-step hydrothermal method for 5-hydroxymethylfurfural electrocatalytic oxidation (HMF-ECO) to high-valued 2,5-furandicarboxylic acid (FDCA) for the first time. The results illustrate that Cu can regulate CoCu–CH morphologies from 1D nanorods to 2D ultra-thin nanosheets besides modulating the catalytic compositions . The optimal Co 1 Cu 1 –CH exhibits hybrid nanostructures containing the 1D nanorods and 2D ultra-thin nanosheets , which has the largest ECSA and specific surface area, as well as the smallest Tafel slope and impedance. The oxidation potential of HMF-ECO is 1.42 V vs RHE with the conversion of HMF 99.57%, the selectivity for FDCA 99.91%, and the FE 98.88%. In addition, Cu can promote the conversion of Co 2+ to the favorable Co 3+ for HMF-ECO on the catalyst surface . Density functional theory calculation indicates that Cu can improve charges transfer to HMF and lower its adsorption energy . In situ Raman spectra tests indicate that cobalt species is the active site for HMF-ECO. Furthermore, at 1.42 V vs RHE, the coupling of HMF-ECO and hydrogen evolution reaction shows that the cathodic hydrogen evolution rate is 92.33 L h −1 m −2 , which is 3.69 times more than water splitting. This work provides a special structures material to process intensification of HMF electrooxidation coupling hydrogen production .
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2023
·
IF 6.8
Yirong Zhang,Zhenchao Tan,Kaikai Qin,Chenglan Liu
Pesticides and heavy metals commonly coexist in soil. In this study, the influence of Cd and Cu on the toxicity of rac -dinotefuran and the enantioselective behavior of dinotefuran enantiomers in soil-earthworm microcosms were investigated. The acute toxic tests showed that S -dinotefuran has higher toxic than that of R -dinotefuran. The rac -dinotefuran and Cd has an antagonistic effect on earthworms, and the Cu and rac -dinotefuran has a synergistic effect. Earthworms maybe promoted the enantioselective behavior of dinotefuran in soil. Co-exposure to Cd or Cu inhibited the dissipation of dinotefuran enantiomers ( S -dinotefuran and R -enantiomers), and slightly reduced the enantioselectivity in soil. The earthworms were found to be preferentially enriched with S -dinotefuran. However, Cd or Cu attenuated the accumulation of dinotefuran enantiomers in earthworms and decreased the enantioselectivity. The effect of Cd and Cu on the environmental behaviors of dinotefuran enantiomers were correlated positively with the dose of Cd/Cu. These results showed that Cd and Cu alter the environmental behaviors and the toxicity of dinotefuran enantiomers in soil-earthworm microcosms. Thus, the influence of coexistent heavy metals on the ecological risk assessment of chiral pesticides should be considered.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 32
·78988-79000
·
IF 5.8
Dong Jiayu,Song Xianni,Zhang Shuchi,Tan Mengyu,Zhao Haiyan,Wu Donglei
A novel hierarchical Cu/ZSM-5 was prepared over alkaline treatment and incipient wet impregnation method for the catalytic ozonation of polyvinyl alcohol (PVA). Under the optimum preparation conditions, hierarchical Cu/ZSM-5 exhibited an excellent mineralization performance during the PVA degradation process, and the removal rate of TOC after 60 min of reaction was 47.86%, much higher than that of ozonation alone (5.40%). Its high catalytic activity could attribute to the large pore volume (0.27 cm 3 /g) and pore size (6.51 nm) which are beneficial for the distribution of loaded copper and adsorption performance for PVA. Compared to ·OH, 1 O 2 (2.66 times in 10 min) contributed more to the removal of PVA. The degradation of PVA was a combined process of direct ozone oxidation, catalytic ozonation and adsorption. With its high catalytic performance and stability, hierarchical Cu/ZSM-5 has a very broad application prospect in the process of catalytic ozonation of refractory pollutants.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Huiqian Yang,Min Wang,Tingting Yang,Chunxia Li,Aifeng Li,Jinsheng Zhao
This paper mainly uses the molecular recognition principle and synergistic effect to synthesize the functional supramolecular 2,7-bis(4-([2,2':6',2''-terpyridin]-4'-yl)phenyl)-9-(heptadecan-9-yl)-9 H -carbazole. The nitrogen active sites at both ends of terpyridine are coordinated with metal copper ions to form a metal supramolecular catalyst that contains both the metal and nitrogen active sites. The surface physical structure and elemental analysis of the synthesized complexes were analyzed using SEM and XPS. The redox properties of the catalysts were characterized using chemical characterization methods, such as cyclic voltammetry (CV), linear sweep voltammetry (LSV), and a rotating ring disk electrode (RRDE). The physical and chemical analysis showed that the catalyst was successfully synthesized and that it was subjected to a redox reaction via a four-electron process. Therefore, the prepared metal supramolecular catalyst has good catalytic performance.
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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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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Weidan Na,Changjin Ou,Yijun Ming,Yuchong Gao,Lin Tian
Surface enhanced Raman spectroscopy (SERS) detection was not as accurate and reproducible as fluorometry due to some uncertainties such as operator's focus adjustment and difference between capillaries. Herein, the weak Raman signal (1640 cm −1 ) from water bending vibration is adopted as a benchmark to improve the practical applicability of Raman detection. Specifically, amygdalin and citrate sodium were applied as reducing and capping agent to synthesize dual-ligand gold nanoparticles (DL-AuNPs). Additionally, the cyano group of amygdalin can attach to the surface of DL-AuNPs and generate a primary SERS signal (2174 cm −1 ), which can be significantly enhanced by Cu(II) as DL-AuNPs aggregates. More importantly, the strong binding affinity between pyrophosphate ions (PPi) and Cu(II) redisperses DL-AuNPs and decreases the signal intensity, making the DL-AuNPs/Cu(II) SERS sensor promising for the detection of PPi. This proposed method presents a reliable SERS analysis with the stable water background calibration and broaden the application of SERS technique in aqueous solution target monitoring.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 14
·4045-4053
·
IF 7
Zhaoguo Hong,Xin You,Jingjing Zhong,Di Yao,He-Dong Bian,Shulin Zhao,Liangliang Zhang,Hong Liang,Fu-Ping Huang
Chemodynamic therapy (CDT), in which highly toxic hydroxyl radicals (˙OH) could be triggered by a Fenton or Fenton-like reaction to kill cancer cells, has emerged recently. Compared to traditional CDT nanomaterials, herein, an atomically-precise biotinylated Cu(I/II) complex [CuICuIICl2(VBio)]·CH3OH (VBio = deprotonated O-vanillin biotinylhydrazone), denoted VBio-CuICuII, was rationally designed and synthesized successfully. This targeted Fenton-like agent, VBio-CuICuII, is constructed from a hydroxyl radical-producible CuI ion, a CuII center as a GSH depletor for an augmented CDT effect, and a biotin moiety as a cancer-targeting unit. Owing to the obvious cell selectivity discrepancy of biotin towards normal and cancerous cells, VBio-CuICuII was able to preferentially accumulate in tumor cells. Meanwhile, the CuI metal center could be used as a Fenton-like agent to generate ˙OH. Furthermore, the CuII in VBio-CuICuII was available for successive ˙OH production via a CuI/CuII-circulation strategy under a GSH-rich tumor site, thereby improving catalytic efficiency. More importantly, in vivo results further demonstrate that VBio-CuICuII could significantly inhibit tumor growth without obvious damage toward major organs. Therefore, this multiple-identity Fenton-like agent could provide an appreciable reference value for the design of atomically precise CDT agents.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Pengtao Sheng,Youyang Xie,Shuyu Han,Yanling Li,Weili Li
Manganese ion-doped quantum dots (QDs) with wide band gaps have been widely investigated to modify their electronic, magnetic, and photophysical properties. The research on Mn-doped Cu-In-Se QDs with narrow band gaps has been minimal due to the profound differences in the reaction reactivity of cations. In this work, photoluminescent and magnetic Cu-In-Se QD nanoprobes were designed and synthesized by introducing Zn 2+ ions, which function as an intermediate acid that can regulate metal ion acidity to enhance the doping efficiency of Mn 2+ ions in a facile phosphine-free hot-injection protocol. The emission peaks of Zn-doped Cu-In-Se QDs and MnZn-doped Cu-In-Se QDs exhibit significant composition-dependent shifts. Moreover, incorporating manganese ions confers a paramagnetic character to MnZn-doped Cu-In-Se QDs and provides a quasi-core shell structure with an Mn-rich alloy shell layer, as demonstrated by the micro-structural surface analysis and electron paramagnetic resonance spectroscopy . Analyzing the decay lifetime and quantum yield reveals that this host-dopant coupling involves a preferential energy transfer from the host material to the dopant (Mn 2+ ions), wherein photogenerated electrons nonradiatively transfer to the 4 T 1 level of Mn dopant and then recombine with the Cu x state above the valance band of host QDs. The ability to serve as nanoprobes for the visualization of tumors through fluorescence and magnetic resonance dual-modality imaging makes these ternary MnZn-doped Cu-In-Se QDs strong candidates for practical applications in biology/biomedicine field.
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VACUUM
·
2023
·
IF 4
Jian Zhang,Chang Xu,Jing Li,Huanjun Lu,Shaohui Zhang,Chao Wang
In this paper, the Cu-/Ni-based one-dimensional (1D) conductive metal-organic frameworks (c-MOFs) nanorods (Cu 3 (HHTP) 2 /Ni 3 (HHTP) 2 ) have been synthesized successfully through a one-pot hydrothermal method . The effect of reaction time, MOFs compositions and ratio of solvent on the performance of Cu 3 (HHTP) 2 -/Ni 3 (HHTP) 2 - based resistive temperature sensors was studied by sensing platforms. Compared with Ni 3 (HHTP) 2 -based sensor, Cu 3 (HHTP) 2 -based sensor, which was assembled under DMF volume of 0.5 mL and reaction time of 12 h (Cu7), provided the optimal performance, for example, relative variation of resistance (RVR) near-linearly decreased by 85.9% from 20 °C to 80 °C, and the temperature coefficient of resistance (TCR) reached up −0.0157 °C -1 . Moreover, the resistance value of the Cu 3 (HHTP) 2 -based sensor is 0.106 kΩ, which exhibited a minimum resistance under different temperatures. These results demonstrate that the use of Ni 3 (HHTP) 2 -based 1D c-MOFs for fabrication of temperature sensor provides good conductivity and high thermo-responsive sensitivity. Hence, this study provided an excellent example for the simple preparation and practical application of 1D c-MOFs-based near-linear temperature sensor.
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