ACS Omega
·
2025
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IF 4.3
Xiaoyan Wang,Xiao Wang,Wanke Chen,Jing Yuan,Qianfeng Zhang
In this study, straw biochar (TB) was prepared by pyrolysis at 500 °C, and biochar composite material (TBS) was prepared by a 1:4 mass ratio with sludge (TS). Scanning electron microscopy and Fourier transform infrared spectroscopy were utilized to characterize the material before and after adsorption. The results demonstrated that TBS possesses significant pore structure characteristics and abundant active functional groups such as hydroxyl, carboxyl, and carbonyl groups, providing a structural basis for its efficient adsorption of heavy metal ions in aqueous solutions. The adsorption performance of the remediation materials for Cu(II) and Pb(II) in aqueous solution was systematically investigated. Experimental data showed that TBS achieved maximum adsorption capacities of 60.86 and 46.98 mg/g for Cu(II) and Pb(II) at equilibrium, respectively, exhibiting superior adsorption efficiency. Through fitting analysis using adsorption kinetic models and isothermal adsorption models, it was found that the pseudo-second-order kinetic model and Freundlich isothermal model could more accurately describe the adsorption process of the two heavy metal ions, indicating that chemical adsorption was the dominant mechanism and characterized by multilayer adsorption. Thermodynamic parameter calculations revealed negative ΔG values and positive ΔH and ΔS values, suggesting that the adsorption process was a spontaneous, entropy-increasing, and endothermic reaction. These research results fully validate the excellent removal capabilities of TBS for Cu(II) and Pb(II). This study has shown that TBS can be considered a promising and cost-effective adsorbent, demonstrating its potential to adsorb heavy metal ions in water.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2022
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IF 9.221
Xian-En Zhao,Ya-Nan Zuo,Yinghui Xia,Jing Sun,Shuyun Zhu,Guobao Xu
Although fluorescent nanozymes exhibit great potential in sensing fields, few current nanozyme-based sensors are designed to discriminate catechol (CC) from its two isomers. Herein, fluorescent metal-organic framework (MOF)-based nanozyme is utilized for ratiometric and selective detection of CC without the interferences of hydroquinone (HQ) and resorcinol (RC). NH 2 -Cu-MOF plays multiple roles: (1) it exhibits excellent photoluminescence at 435 nm owing to the 2-amino-1,4-benzenedicarboxylic acid ligand; (2) Cu 2+ imparts MOF oxidase activity to trigger the oxidation of o -phenylenediamine (OPD) into luminescent products (oxOPD) with emissive peak at 571 nm, which quenches the intrinsic fluorescence of NH 2 -Cu-MOF (435 nm) through inner filter effect (IFE); (3) Cu 2+ can complex with CC specifically to produce complex containing o -semiquinone, which not only inhibits MOF’s oxidase-like activity but also quenches the fluorescence of MOF. Therefore, the presence of CC induces the decrease of fluorescence at 571 nm followed by the slight recovery of fluorescence at 435 nm. Notably, HQ and RC have negligible influences on the fluorescence of NH 2 -Cu-MOFs/OPD system. Based on these facts, a ratiometric fluorescence platform for CC has been constructed. It exhibits high sensitivity towards CC with LOD of 0.1 μM.
研究领域:
分析化学
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生物传感
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材料科学
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DOI
高影响因子
JOURNAL OF POLYMERS AND THE ENVIRONMENT
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2024
·Vol. 32
·期 7
·3326-3341
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IF 4.7
Wang Rui,Song Xin,Liu Li,Zhou Chao,Wu Guangfeng
Magnetic particles with active groups on their surfaces can be applied to wastewater purification to remove harmful ions, but the insufficient number of active groups on their surfaces tends to limit their removal rate of ions. Herein, we grafted different generations of dendritic macromolecular polyamidoamine (PAMAM) onto the magnetic chitosan microspheres (MCS) using ethylenediamine tetraacetic acid (EDTA) as core (MCEPs) for the removal of Cu (II). Firstly, 7 μm-sized MCS with good dispersibility was prepared by adjusting conditions such as glacial acetic acid content, emulsifier content and raw material ratio. Secondly, the effect of MCEPs generation, pH and contact time on the adsorption capacity were investigated. The adsorption experiments showed that the MCEPs had a high adsorption capacity, when the adsorbent was the second generation of MCEP (MCEP G2.0), the maximum adsorption capacity can up to 702.9 mg/g and the adsorption process can be completed in 60 min. Moreover, among various isotherms models, MCEP G2.0 was well-fitted by Langmuir adsorption isotherm. Also, adsorption kinetic studies proved that the adsorption mechanism of MCEP G2.0 adsorbent followed the pseudo-second-order kinetic model, demonstrating that the process was chemisorption. The adsorbent has renewability as well, after five adsorption cycles, its adsorption efficiency was still higher than 80%. Therefore, the adsorbent showed a superior adsorption capacity and renewability to remove Cu (II). Graphical
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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DOI
高影响因子
ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Yuan Qin,Huimei Liang,Jia Wu,Zheyang Chi,Shulin Zhao,Fanggui Ye
Natural enzyme cascades, including the same and different kinds of enzymes, have been widely used in biosensing. However, it is still a challenge for nanozymes, the mimics of natural enzymes, to achieve biosensing with different types of enzyme-like activities based on cascade reactions, such as hydrolase and oxidoreductase. Considering the characteristics of the multienzyme-like activity of some nanozymes, as a proof of concept, this study demonstrates a Cu/Ce-MOF-808 nanozyme as a self-cascade catalyst with hydrolase-like and catechol oxidase-like activities. Taking organophosphorus pesticides as an example, we constructed a self-cascade catalytic reaction for the one-step colorimetric detection of isocarbophos. Specifically, the hydrolase-like activity of Cu/Ce-MOF-808 can hydrolyze isocarbophos to produce colorless isopropyl salicylate, which is further oxidized by the catechol oxidase-like activity of Cu/Ce-MOF-808 and complexed with 4-aminoantipyrine (4-AAP) to produce red quinoneimine under neutral conditions with illumination. Thus, a colorimetric strategy for sensitive isocarbophos analysis is developed, with a linear range of 0.90–400.00 μg·mL–1 and a detection limit of 0.42 μg·mL–1. This research presents a new approach to the design and synthesis of nanozymes and has great application potential in the field of nanozyme cascade biosensing.
研究领域:
生物化学
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纳米生物学
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分析化学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Yifan Li,Jiaxing Li,Lin Chen,Yunpeng Long,Xing Yuan,Junhua Li,Yue Peng
The low selectivity for N2 in the oxidation of NH3 over commercial Pt/Al2O3 catalysts is primarily due to the overoxidation of NH3 facilitated by Pt sites, leading to the formation of unwanted byproducts such as N2O and NO. In this study, we present a novel strategy to enhance N2 selectivity while maintaining NH3 conversion by constructing Pt–O–Cu dual sites. These dual sites exhibit synergistic acid-redox characteristics through surface electron transfer mediated by bridged lattice oxygen. Additionally, the ability of surface-adsorbed oxygen to exchange with lattice oxygen is significantly improved. The electron-deficient Cu sites enhance NH3 adsorption by providing empty 3d orbitals, while the electron-rich Pt sites promote NH3 dehydrogenation. Subsequently, the formation of –NH or –N intermediates at the Pt sites can react with adsorbed NH3 on the Cu sites to produce N2, predominantly following the integrated selective catalytic reduction mechanism. The optimized dual-site catalyst achieves over 95% NH3 conversion and N2 selectivity at 180 °C.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Qiaohong Su,Qingcui Liu,Pengyue Wang,Juan Ding,Jiulin Wang,Yudai Huang
High overpotential and low stability are major challenges for hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). Tuning the electronic structure of catalysts is regarded as a core strategy to enhance catalytic activity. Herein, we report CuO x /Cu nanorod skeleton supported Ru doped cobalt oxide/nitrogen-doped carbon nanocomposites (Ru-CoO/NC/CuO x /Cu, denoted as RCUF) as bifunctional catalysis. The one-dimensional/three-dimensional (1D/3D) nanostructure and defect-rich amorphous/crystalline phases of RCUF facilitates active site exposure and electron transport. Experimental characterization and density functional theory (DFT) calculation results indicate that Ru doping can optimize the electronic structure, which accelerates the water dissociation process and reduces the Gibbs free energy of the reaction intermediates. As expected, the optimal RCUF-900 exhibits low overpotential (25/205 mV at 10 mA cm −2 ) and high stability (100/100 h) for HER/OER. RCUF-900 has low voltage (1.54 V at 10 mA cm −2 ) and high stability (100 h) for overall water splitting. This work provides new insights into the design of advanced catalysts for overall water splitting.
研究领域:
材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Fangyi Pei,Zhimiao Wang,Jianhua Lv,Fang Li,Wei Xue
Cu–Zn–Al catalyst was prepared by the co-precipitation method, and the catalytic performance for transfer hydrogenation of acetophenone (AP) to 1-phenylethanol (1-PhE) was evaluated using isopropanol (IPA) as a hydrogen source. The addition of Zn changed the morphology of the catalyst and reduced aggregation of catalyst particles, resulting in highly dispersed Cu active sites. As the Zn content increased, the valence state of Cu species changed. When the Cu/Zn molar ratio was 2/3, the Cu+/Cu0 ratio in the catalyst was 0.81, resulting in good selectivity for 1-PhE. The reaction conditions were optimized over the Cu–Zn–Al catalyst with a Cu/Zn molar ratio of 2/3. When the reaction was performed at 180 °C for 2 h with an IPA/AP molar ratio of 15, the AP conversion was 89.4% and the 1-PhE selectivity was 93.2%. The Cu–Zn–Al catalyst showed good stability, and AP conversion and the 1-PhE selectivity were essentially unchanged after five cycles.
研究领域:
催化化学
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有机合成
·
材料科学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
·
IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
研究领域:
材料科学
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催化化学
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能源转换
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DOI
高影响因子
Materials Today Physics
·
2022
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IF 11.021
X. Li,Z. Wang,J. Zhang,K. Dai,K. Fan,G. Dawson
The solar driven reduction of carbon dioxide (CO 2 ) to high value-added carbon based fuel is a promising solution to mitidate climate and energy problems, however, improving the adsorption and conversion efficiency of CO 2 in the photoreduction process still faces severe challenges. In this work, Cd 0·7 Zn 0·3 Se solid solution was prepared by cation exchange: selenium (Se) vacancies are produced during ion exchange, which promotes the unsaturated coordination of the surrounding metal atoms. The adsorption of diethylenetriamine (DETA) on the surface limits the growth of Cd x Zn 1- x Se crystallites , resulting in insufficient coordination of the surface atoms, which then become active adsorption sites. Furthermore, a heterojunction was formed with Cu 2 O@Cu to accelerate the separation and transfer of photo-induced carriers of Cd 0·7 Zn 0·3 Se, and the optimized Cd 0·7 Zn 0·3 Se/Cu 2 O@Cu (CZS/CC) step-scheme heterojunction exhibited a CO release activity of 50.5 μmol g −1 h −1 , which is 3.8 and 10.7 times higher than that of Cd 0·7 Zn 0·3 Se and Cu 2 O@Cu, respectively. This work is expected to open up new insight for the regulation of nanostructures and the design of selective catalysts.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Minglei Lu,Zhuoyu Zheng,Weiwei Lu,Haiping Zhu,Junwei Liao,Yuxin Ge,Xueer Huang,Qian Zhang,Jiajin Li,Yiyuan Zhou,Xiaoping Wu,Baozhu Chen,Chunxiao Yang,Xitang Qian,Minhua Shao,Tiejun Wang
Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H2) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu2O, and CuN3 nanoparticles anchored on the nitrogen-doped carbon, forming Cu0/Cu+/Cu-N3 active sites. This catalyst achieves a H2 production rate of 140.1 μmol/gcat/s at 210 °C, which is several times to 2 orders of magnitude higher than that of Cu-, Ni-, even Pt-based catalysts, demonstrating excellent long-term stability over 350 h at 210 °C. A mechanism investigation reveals that the Cu-N3 site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H2 production kinetics.
研究领域:
催化化学
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能源材料科学
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产品关联
DOI
PubMed
高影响因子
Chem Catalysis
·
2022
·
IF 0
Wenjie Wu,Yulu Yang,Yitong Wang,Tiantian Lu,Qingsong Dong,Junwei Zhao,Jingyang Niu,Qingchao Liu,Zhaomin Hao,Shuyan Song
Electrosynthesis of urea from N 2 and CO 2 molecules is of immense significance but has so far been plagued by the lack of a universal design principle to guide the search for new catalysts. Herein, as exemplified by the Cu-Bi catalyst, our findings revealed that the defective Cu-Bi catalyst could offer a maximum urea concentration of 0.45 ± 0.06 mg L −1 and the largest faradaic efficiency of 8.7% ± 1.7% at −0.4 V (versus reversible hydrogen electrode [RHE]), exhibiting outstanding activity in contrast to monometallic (Cu and Bi) and bimetallic (Cu-Bi mixture and intact Cu-Bi) catalysts. Moreover, the evidence from isotope tracing experiments, in situ Raman spectroscopy, and density functional theory (DFT) calculations suggested that it is a promising strategy for the co-reduction of N 2 and CO 2 by defective Cu-Bi catalysts, switching on a light to the application of defects in electrosynthesis of urea.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
DOI
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huijuan Chen,Fangrui Gao,Wenbin Ren,Lulu Du,Kaifeng Xue,Pinhua Zhang,Changmin Shi,Li Lv,Guangliang Cui
Ultra-sensitive hydrogen sulfide (H 2 S) detection technology at low temperatures provides critical support for the application of one-time alert systems under extreme conditions, ensuring reliable monitoring of H 2 S in low-temperature environments and enhancing safety and practicability. In this study, we developed a novel low-temperature H 2 S sensor based on Cu/Cu 2 O nanoarrays, prepared through a combination of 2D electrodeposition in situ assembly and the hydrothermal method. The heterointerface between Cu nanowires and Cu 2 O nanocubes presents a high barrier, which can be modulated to zero through the formation of continuous Cu x S conductive channels via the vulcanization reaction, thereby achieving excellent sensitivity and selectivity towards H 2 S at low temperatures. At freezing temperatures and low H 2 S concentrations (≤20 ppm), the sensors show ideal recovery and reasonable sensitivity (R=150 to 10 ppm H 2 S at 0 °C). However, the response significantly increases (R=5624 at 10 ppm H 2 S at 50 °C) and recovery is lost under reversed conditions. First-principles calculations have confirmed that the enhanced H 2 S adsorption at the heterointerface is the primary reason for the robust response observed at 0 °C. Experimental results demonstrate that the Cu/Cu 2 O nanoarrays were capable of rapid detection of H 2 S at low temperatures through modulation of heterointerface barriers.
研究领域:
材料科学
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化学传感器
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表面科学
✓ 已验证
产品关联
DOI
高影响因子