JACS Au
·
2025
·
IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chenxu Guo,Miao Li,Wenming Guo,Jiawei Xie,Hang Qin,Moyu Liao,Yi Zhang,Pengzhao Gao,Hanning Xiao
Methanol steam reforming (MSR) is considered as a promising approach to provide hydrogen for proton-exchange membrane fuel cells. However, it is challenging to develop effective and durable Cu-based catalysts. Herein, Cu-ZnO catalysts are prepared by facile quenching of ZnO in copper nitrate solution followed by reduction to obtain the desired metal loading and induce the doping of surface metal heteroatoms for producing more vacancies. Catalysts enriched with oxygen vacancies can efficiently activate H 2 O and rapidly transform C-containing intermediates, resulting in higher methanol conversion and lower CO selectivity. As a result, the quenched optimal catalyst achieves 100 % methanol conversion and 0.05 % CO selectivity at 280 ℃, exhibiting the excellent catalytic performance in MSR reaction. In practical applications, structured catalysts are more attractive for large-scale catalytic reactions owing to the low pressure drop and high utilization efficiency. Therefore, ZnO-Cu 3 catalyst is coated on cordierite honeycomb ceramics with 100 % methanol conversion and 0.04 % CO selectivity at 280 ℃. After 100 h of the reaction, the structured catalyst remains ∼ 92.3 % with CO selectivity varying from 0.02 to 0.06 %, demonstrating the good catalytic stability in the long-term experiment. In addition, the evolution of reactants and intermediates on the catalyst surface are briefly described by FTIR spectra. This study offers a novel and efficient approach to obtain highly active and durable catalysts with great potential for industrial-scale preparation and application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Haitao Yan,Didi Li,Zhaocong Jiang,Haoyuan Gu,Mengyuan Zhu,Yi-Fan Han,Minghui Zhu
Cu-based catalysts have been extensively used in the methanol steam reforming (MSR) reaction owing to low cost and high efficiency. In this work, we investigated the promotional effect of Fe on the Cu/ZnO/Al 2 O 3 catalysts prepared by an incipient-wetness impregnation method using a series of (quasi) in situ characterization techniques. The form of the Fe species was found to strongly depend on the Fe content. Fe species are present as highly dispersed FeO x in small amount of Fe with improved the dispersion of Cu. As Fe content increases, Fe species gradually transition to CuFe alloy and eventually to Fe 3 O 4 particles, leading to a decrease in Cu dispersion. With the gradual increase in Fe content, the apparent activity shows a volcanic trend, with CuAl-0.1Fe showing highest activity, whereas the intrinsic activity gradually decreases. Compared with CuAl- x Fe, adding moderate Fe to Cu/ZnO/Al 2 O 3 promotes the dispersion of Cu and Zn, forming abundant Cu-ZnO x interfacial sites, which improves both apparent and intrinsic activities. The best catalytic performance was obtained with the CuZnAl-0.1Fe catalyst, achieving the highest H 2 production rate of 134.7 mmol g cat −1 h −1 at 200 °C. This study reveals the role of Fe in Cu-based catalysts for MSR and inspires the design of improved Cu-based catalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 50
·e07124
·
IF 19
Xibei Jia,Xiaobo Wu,Long Qi,Xianggang Dai,Jian Wang,Tao Jiang,Zhanyong Hong
In the context of the ongoing development of artificial intelligence and 5G technologies, a growing number of sensors are being integrated into the daily lives. Self-powered wearable sensors based on triboelectric nanogenerator (TENG) represent an innovative solution to this trend, but the output performance of the flexible TENGs remains suboptimal. In this study, the band-matched calcium titanate (CaTiO 3 ) and zinc oxide (ZnO) nanostructures are prepared to form CaTiO 3 /ZnO (CTO/ZnO) Schottky heterojunctions. The heterojunctions are subsequently doped into organic ferroelectric polyvinylidene fluoride (PVDF) to create flexible composite film, which significantly increases the dielectric constant through space charge polarization. Then the CTO/ZnO-PVDF composite films served as triboelectric materials of the CaTiO 3 /ZnO-PVDF-based TENG (CZP-TENG). After optimizing the molar ratio of ZnO to CTO in heterojunction and weight ratio of CTO/ZnO in PVDF, both the output voltage and current density of the TENG are significantly improved, exhibiting a power density of 106.6 mW m −2 . Finally, the CZP-TENG powers light–emitting diodes and a temperature sensor, serves as a wearable sensor, and enables self-powered human body sensing, particularly in gait recognition for preventing of movement-related diseases and injury rehabilitation.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 64
·e202201682
·
IF 5.02
Longbin Xian,Nanlin Zhang,Zufu Luo,Xiaolin Zhang,Chonglin Yuan,Xiuting Li
Graphical Cyclic voltammetry (CV) is employed to determine the band edges and trap states of ZnO QDs with different surface ligands. It is demonstrated that the ZnO QDs without surface ligands mainly have oxygen interstitial defects whilst the ZnO QDs covered with ligands contain oxygen vacancies. The electronic structure of quantum dots (QDs) including band edges and possible trap states is an important physical property for optoelectronic applications. The reliable determination of the energy levels of QDs remains a big challenge. Herein we employ cyclic voltammetry (CV) to determine the energy levels of three types of ZnO QDs with different surface ligands. Coupled with spectroscopic techniques, it is found that the onset potential of the first reductive wave is likely related to the conduction band edges while the first oxidative wave originates from the trap states. The determined specific energy levels in CV further demonstrates that the ZnO QDs without surface ligands mainly have oxygen interstitial defects whilst the ZnO QDs covered with ligands contain oxygen vacancies. The present electrochemical method offers a powerful and effective way to determine the energy levels of wide bandgap ZnO QDs, which will boost their device performance.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Obeng Enoch,Feng Jiayao,Wang Danyan,Zheng Dongyang,Xiang Bailin,Shen Jianliang
To overcome the limitations of traditional therapeutics, nanotechnology offers a synergistic therapeutic approach for the treatment of bacterial infection and biofilms that has attracted attention. Herein, we report on a ZnO@Ag nanocomposite with good biocompatibility synthesized by doping ZnO NPs with silver nanoparticles (Ag NPs). ZnO@Ag nanocomposites were synthesized with varying ratios of Ag NPs (0.5%, 2%, 8%). Under the same experimental conditions, ZnO@8%Ag exhibited outstanding properties compared to the other nanocomposites and the pristine ZnO NPs. ZnO@8%Ag demonstrated excellent photothermal and photodynamic properties. Also, ZnO@8%Ag demonstrated over 99% inhibition of Staphylococcus aureus (S. aureus) under photothermal therapy (PTT) or photodynamics therapy (PDT) as a result of the excessive generation of reactive oxygen species (ROS) by the Ag+ released, while the pristine ZnO showed an insignificant inhibition rate compared to the PBS group (control). Furthermore, ZnO@8%Ag completely disrupted S. aureus biofilm under a combined PTT/PDT treatment, a synergetic trimodal therapy, although the molecular mechanism of biofilm inhibition remains unclear. Hence, the excellent photothermal, photodynamic, biocompatibility, and bactericidal properties of ZnO@8%Ag present it as an appropriate platform for bacterial and biofilm treatment or other biomedically related applications.
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SURFACE & COATINGS TECHNOLOGY
·
2021
·
IF 4.158
Zefei Yu,An Du,Chenyang Wang,Ruina Ma,Yongzhe Fan,Xue Zhao,Xiaoming Cao
Herein, a ZnO-doped plasma electrolytic oxidation (PEO) composite coating was prepared on the surface of a 1060 Al alloy by adding ZnO nanoparticles (ZnO-NPs) to the composite electrolytes of alkaline sodium silicate (Na 2 SiO 3 ) and sodium hexametaphosphate ((NaPO 3 ) 6 ). To efficiently investigate the coating's microstructure, the detached PEO coating was prepared without damage via an electrochemical method. The morphology and phase composition of the PEO coating were analyzed using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), transmission electron microscopy (TEM), and X-ray diffraction (XRD), and an incorporation model of ZnO-NPs was established. The results showed that the addition of ZnO-NPs slightly prolonged the anodic oxidation time and increased the breakdown voltage, whereas the working voltage and final voltage decreased slightly. The XRD results indicated that although the addition of ZnO-NPs did not result in the production of Zn-containing phases, it affected the formation and transformation reactions of other phases. SEM micrographs of the fractured cross-section of detached coating and coating/substrate interface indicated that the ZnO-NPs did not enter the interface layer, nor did it participate in the formation of the cap structure at the interface. Based on the experimental results and the “cascade discharge” model, an incorporation model of ZnO-NPs in PEO has been proposed.
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JOURNAL OF CULTURAL HERITAGE
·
2019
·
IF 1.955
Minghao Jia,Xiaogang Zhang,Jiajia Weng,Jie Zhang,Meifang Zhang
Coating of ZnO-cellulose composites on paper surface has potential technological applications. With this motivation, a simple approach of synthesizing ZnO nanoparticles in cellulose nanocrystals (CNC) by in-situ solution casting is reported in this work. The surface morphology of ZnO nanoparticles combined with cellulose fibers and the distribution of these ZnO-cellulose composites on the paper surface were characterized by scanning electron microscopy. The results showed that ZnO nanoparticles are easily and uniformly dispersed in the CNC. The ZnO-cellulose composite nanofluids were prepared by dispersing the composites in isopropanol as a base fluid. To determine the protective potential of these coatings, the chemical and mechanical properties of coated papers after dry heat and UV accelerated aging were measured. Also, a good color stability of the paper coated by the nanocomposites was observed through colorimetric measurements . The paper coated with ZnO-cellulose composites was found to possess antibacterial and antifungal activity against five common fungi (Aspergillus niger, Aspergillus Versicolor, Rhizopus nigricans, Saccharomycetes, Mucor) observed in the archive or museum and two bacteria (Staphylococcus aureus and Escherichia coli) in common life.
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ACS Applied Materials & Interfaces
·
2013
·
IF 5.008
Yuyu Bu,Zhuoyuan Chen,Weibing Li,Baorong Hou
In the present paper, the graphene–ZnO composite with quasi-shell–core structure was successfully prepared using a one-step wet chemical method. The photocatalytic Rhodamine B degradation property and the photoelectrochemical performance of the graphene–ZnO quasi-shell–core composite are dependent on the amount of graphene oxide that is added. When the amount of graphene oxide added is 10 mg, the graphene–ZnO quasi-shell–core composite possesses the optimal photocatalytic degradation efficiency and the best photoelectrochemical performance. An efficient interfacial electric field is established on the interface between the graphene and ZnO, which significantly improves the separation efficiency of the photogenerated electron–hole pairs and thus dramatically increases its photoelectrochemical performance. In addition to the excellent photocatalytic and photoelectrochemical properties, the electron migration ability of the grephene–ZnO quasi-shell–core composite is significantly enhanced due to the graphene coating on ZnO surface; therefore, this material has great potential for application as a substrate material to accept electrons in dye solar cell and in narrow bandgap semiconductor quantum dot sensitized solar cells.
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Environmental Science-Nano
·
2019
·Vol. 7
·期 1
·327-338
·
IF 7.704
Tao Wang,Yangyang Liu,Yue Deng,Hanyun Cheng,Yang Yang,Kejian Li,Xiaozhong Fang,Liwu Zhang
Atmospheric photochemistry is widely regarded as an important pathway for SO2 oxidation. The influence of irradiation intensity, especially photochemistry under weak sunlight during heavy haze events is not known. This work investigates the irradiation-intensity-dependence of the dust-related heterogeneous process using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and ex situ flow reaction. Illumination of the particles alters the surface oxygen species, and further accelerates the significant oxidation of sulfite species to sulfate products. The sulfate formation rate grows rapidly from the dark state to faint irradiation, while it becomes insensitive to irradiation intensity variation under strong illumination. According to the photo-electrochemical tests and concentration dependence experiments, this interesting phenomenon can be interpreted by the presence of excess SO2 under weak sunlight and sufficient photoinduced active species (PAS) under strong illumination. This uneven promotion effect is beneficial for explaining the sulfate burst under faint sunlight during heavy haze events. More significantly, the uptake of SO2 accounts for the increase of acidic species and the decrease of adsorbed water on the particle surface, thus elevating the particle acidity. Under these circumstances, the dissolution of zinc oxide (ZnO) takes place, and results in diverse principal products varying with the illumination condition, e.g. ZnSO3 under weak sunlight while ZnSO4 under strong irradiation. In general, photochemistry has profound impacts on atmospheric sulfur cycling, as well as the cycle of metal elements. The irradiation intensity dependent effects imply the raising uncertainty in the current air quality models.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2019
·Vol. 35
·期 5
·924-928
·
IF 1.071
Xiang Siyuan,Meng Qingnan,Zhang Kai,Gu Yue,Liu Wendong,Yang Bai
Using dextran as both reductant and stabilizing agent, nanopetals(ZnO-Au NPs) were easily synthesized and possessed a petal-like morphology. The feature structure and size of such ZnO-Au NPs were adjustable by regulating the amount of chloroauric acid(HAuCl 4 ). Moreover, the electrochemical property of the obtained NPs was evaluated by being immobilized on the glassy carbon electrode(GCE), which performed both high sensitivity and stability in dopamine(DA) determinations. Furthermore, the as-prepared ZnO-Au NPs could also detect DA and uric acid(UA) simultaneously in the mixture without interference, indicating good selectivity and showing promising potential in biosensing.
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Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Yulin Ma,Mingming Liu,Yange Feng,Hongyu Zheng,Yongling Wu
Piezoelectric polyvinylidene fluoride (PVDF) based piezoelectric materials are good candidates for energy harvesting devices and sensing systems. Improving the piezoelectric sensitivity of the electro-spun PVDF fibers is still challenging and highly desirable. In this work, ZnO@Ag nanoparticles were synthesized and utilized as surface modifier to generate a hierarchical structure on the fiber surfaces to construct a flexible and piezoelectric three-phase coupling sensor. The effects of the atomic ratio of Ag:ZnO, surface morphology and particle concentration of ZnO@Ag nanoparticles on the β-phase content, piezoelectricity, wettability and mechanical stability of the sensor device were systematically investigated. The elastic modulus of ZnO@Ag/PVDF membrane is 0.01322 GPa, which is close to that of human skin 0.0188 GPa. Due to synergistic effect of the enhanced electrostatic field polarization and surface hierarchical structure, the ZnO@Ag/PVDF piezoelectricity sensor possessed voltage and current outputs of 15.0 V pp and 1.775 μA respectively, which were 3.5 and 5.4 times higher than pure PVDF-based sensor. The sensitivity of the ZnO@Ag/PVDF nanofiber-based sensor was 2.422 V/kPa, which was 14.4 times higher than that of pure PVDF-based sensor. The sensor has a fast response/recovery time of 30/45 ms. The sensor can accurately detect various physiological strain signals such as cantilever oscillatory excitation, finger press, or walking behavior, and can light-up several light-emitting diodes (LEDs) and charge a capacitor (20 μF) in a short period (2.41 V in 5 Sec). This fiber-based energy harvesting and pressure sensor demonstrates promising applications in self-powered flexible wearable electronic devices in healthcare and home-care fields.
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