Nano Energy
·
2023
·
IF 17.6
Yajie Cheng,Junjie Ma,Huaiqing Luo,Meng Cai,Tangyue Xue,Guanghui Yu,Ziqiu Ren,Yanlin Song,Shou Peng,Yiqiang Zhang
The undesired segregation of inactive secondary phase that randomly distributed across the perovskite film is detrimental to charge-carrier transport dynamics and light stability. However, in-depth studies for understanding the underlying chemical reaction mechanism and the relationship between phase structural configuration and physical properties are still lacking. Herein, the segregation behavior of the inactive secondary phase and the underlying microcosmic mechanism regarding ionic chemical replacement reaction and lattice reconfiguration process are systematically elaborated. A high-quality perovskite-PbI 2 heterojunction film is constructed via converting the three-dimensional PbI 2 photoactive phase into a two-dimensional inactive phase, alleviating the energetic disorder of carrier dynamics and photochemical dissociation. The resultant perovskite solar cells achieve an efficiency of 24.23% with excellent light-resistance. The dissociation energetics of phase dimensional structure is theoretically analyzed. This work provides new insights into crystal structure design for constructing high-quality perovskite heterojunction devices.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wenfei Dong,Guo Chen,Mengyao Ding,Haiyan Cao,Gaoya Li,Meiqing Fang,Wenbing Shi
Nanozyme-based sensing strategy for glucose generally involves a two-step H 2 O 2 -bridged cascade reaction . However, this two-step cascade reaction always shows a limited detection efficiency for glucose, which hardly makes simply operation, rapid detection, and sensitivity all promised. Herein, a novel strategy for one-step glucose detection was proposed based on the efficiently competitive relationship between glucose oxidase catalyzed glucose oxidation and oxidase nanozyme catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB) colorimetric oxidation. As a proof of concept, Co-Nx sites on porous carbon (Co-Nx/PC) derived from ZIF-67 was selected as the oxidase nanozyme with O 2 -sensitive nature, which can activate O 2 to produce 1 O 2 for TMB colorimetric oxidation. In the presence of glucose, the competitive reaction of glucose oxidase catalyzed glucose oxidation occurs, which will obviously inhibit the Co-Nx/PC catalyzed TMB colorimetric oxidation to construct method for glucose detection. The usage of the same reactant O 2 and the production of suppressive H 2 O 2 cause a dual effect to this inhibition. In addition, the available pH range of Co-Nx/PC overlaps with that of glucose oxidase, promising a one pot reaction . The proposed method with Co-Nx/PC as oxidase nanozyme based on one-step competitive strategy for glucose detection possesses high detection efficiency with convenience (one-pot), rapidness (total reaction time of 10 min) and sensitivity (LOD of 0.31 μM) all promised, which is superior among the methods based on two-step one-pot or two-pot cascade strategy. The strategy can be successfully applied into the blood glucose detection in human serums with satisfactory results. Also, the strategy can be scalable to other oxidase nanozyme like Mn 3 O 4 .
研究领域:
生物化学
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医学检测
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 1
·354-363
·
IF 11.9
Yunxiang Zhang,Chenliang Zhou,Shishi Xu,Hazem Abdelsalam,Zhichao Mu,Wei Chen,Zhili Chen,Xiangyu Cheng,Diab Khalafallah,Qinfang Zhang
Numerous studies disclosed that molten salts provide a special liquid reaction environment, accelerate the diffusion rate of active elements, and promote the formation of high-purity materials in the molten-salt synthesis method. Herein, the interlayer halogen-competing reactions between molten salts and halogen layers during the formation of BaBi4TiNbO11X (X = Cl, Br) oxyhalides were discovered for the first time. The liquid environment provided by molten salts can facilitate the full migration of halogen atoms between molten salts and halogen layers and form an even distribution of halogen atoms, which is ascribed to the weak van der Waals forces of the halogen layers between [BaBiO2]+ and [Bi2O2]2+ blocks. By employing this mechanism, BaBi4TiNbO11(Cl1−xBrx) with different x contents could be easily obtained. DFT calculations showed that the mixed halogen oxyhalides, such as BaBi4TiNbO11(Cl0.5Br0.5), introduce new chemical bonds between the O and Bi atoms, which increase their contribution to lowest occupied/unoccupied orbitals, thus regulating the energy band and accelerating the separation and transfer of photogenerated charge carriers. Consequently, the optimized BaBi4TiNbO11(Cl0.5Br0.5) sample showed a superior degradation rate of RhB compared to the traditional P25 photocatalyst, and its O2 evolution performance was also enhanced compared with other blank samples.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Shuhao Hu,Pingan Chen,Xiangcheng Li,Yingli Zhu,Boquan Zhu
SiBCN ceramics have a wide range of applications in the field of high temperature electromagnetic wave (EMW) absorption owing to their excellent EMW attenuation and oxidation resistance. However, excessive SiC and insufficient Si3N4 in the SiBCN ceramics deteriorate the impedance matching characteristics, and weaken the absorption ability for EMW. In this paper, the amount of SiC and Si3N4 is balanced by a competitive reaction strategy, in which HfZr atoms are introduced to modulate the dielectric phases in the SiBCN ceramics. The formation of a HfZrCN compound produces a cage-like structure around Si3N4, inhibiting the reaction of Si3N4 with carbon to form SiC. The appropriate amounts of SiC and Si3N4, and the abundant interfaces and defects jointly enhance the EMW absorption capability by simultaneously improving the impedance matching and attenuation capability. Thus, an effective absorption band of 4.96 GHz (11.20–16.16 GHz) is reached with a thickness of 1.7 mm for the HfZr-SiBCN ceramics. This work provides a new strategy for simultaneously improving the impedance matching and EMW attenuation capability of polymer-derived ceramics by introducing difficult-to-migrate atoms to regulate the content of the dielectric phase.
研究领域:
材料科学
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电磁学
✓ 已验证
产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2015
·
IF 4.074
Guangyang Liu,Tengfei Li,Xin Yang,Yongxin She,Miao Wang,Jing Wang,Min Zhang,Shanshan Wang,Fen Jin,Maojun Jin,Hua Shao,Zejun Jiang,Hailong Yu
A novel fluorescence sensing strategy for determination of atrazine in tap water involving direct competition between atrazine and 5-(4,6-dichlorotriazinyl) aminofluorescein (5-DTAF), and which exploits magnetic molecularly imprinted polymer (MMIP), has been developed. The MMIP, based on Fe 3 O 4 -chitosan nanoparticles, was synthesized to recognize specific binding sites of atrazine. The recognition capability and selectivity of the MMIP for atrazine and other triazine herbicides was investigated. Under optimal conditions, the competitive reaction between 5-DTAF and atrazine was performed to permit quantitation. Fluorescence intensity changes at 515 nm was linearly related to the logarithm of the atrazine concentration for the range 2.32–185.4 μM. The detection limit for atrazine was 0.86 μM (S/N = 3) and recoveries were 77.6–115% in spiked tap water samples.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wenguang Wang,Chao Wang,Yanqiu Zhang,Hanyang Xu,Lu Shao
Advanced monovalent cation exchange membranes (MCEMs) have been applied to extract key monovalent cations (Li + or Na + ) from nature, but it is challenging to design high-performance MCEMs with low membrane area resistance and specific charge properties. Herein, a positively-charged Fe 3+ -bridged pyrogallic/polyethyleneimine membrane (Fe 3+ -bridged PY/PEIM) for efficient Li + /Mg 2+ separation is fabricated through a covalent bond and coordination bond (CB/COB) competitive reaction. Various physicochemical characterizations elucidate that the formation of COBs reduces the reaction sites of PY and PEI molecules for Michael-addition and Schiff-base reactions, which reduces the thickness of the selective layers to reduce the membrane area resistance from 6.58 to 4.83 Ω·cm 2 . A highly positively-charged selective layer caused by unreacted NH 2 groups and Fe 3+ makes the optimal Fe 3+ -bridged PY/PEIM exhibit a superior separation performance (perm-selectivity (Li + /Mg 2+ ) of 45.57 with a Li + flux of 4.61 × 10 −8 mol·cm −2 ·s −1 ). Moreover, the optimal Fe 3+ -bridged PY/PEIM also has excellent separation performance (high Li + flux and perm-selectivity) and operational stability when treating three simulated solutions with different Mg/Li mass ratios and salinities. The new strategy for constructing a thin, defect-free and positively-charged selective layer through a CB/COB competitive reaction can provide new insights for designing high-performance MCEMs towards environmental remediation and energy harvesting.
研究领域:
材料科学
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环境科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Pian Wu,Xiaosheng Ye,Danqi Wang,Fangjie Gong,Xiaoqian Wei,Shan Xiang,Jingwen Zhang,Tianhan Kai,Ping Ding
Selective and sensitive detection of microcystin-LR (MC-LR) is of vital importance because of its high toxicity and broad distribution. Herein, a novel and versatile fluorescence sensor (Cas14-pMOFs fluorescence sensor) was developed by combining the CRISPR/Cas14a system with a 2D porphyrin metal-organic framework nanosheets (2D-pMOFs) for MC-LR determination. The designed CRISPR/Cas14a system was activated by the unbound complementary DNA (cDNA), which was positively correlated with MC-LR concentration. Furthermore, the activated Cas14a protein was utilized to indiscriminately cleave the FAM-labeled single-stranded DNA (ssDNA-FAM), which was pre-absorbed on Cu-TCPP(Fe) nanosheets. Because of the desorption of the cleaved ssDNA-FAM, the pre-quenched fluorescence signal was recovered. Owing to the excellent performance in quantifying cDNA using this Cas14-pMOFs fluorescence sensor with a limit of detection (LOD) of 0.12 nM, this Cas14-pMOFs fluorescence sensor was able to detect MC-LR in a range from 50 pg/mL to 1 μg/mL with the LOD of 19 pg/mL. This work not only provided a new insight for the exploration of fluorescence sensors based on 2D-pMOFs coupled with CRISPR/Cas14a, but also, demonstrated its universality in both nucleic acid and non-nucleic acid targets determination.
研究领域:
分析化学
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生物技术
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 110
·108791-108800
·
IF 3.289
Wei Zhou,Haiqian Zhao,Jihui Gao,Xiaoxiao Meng,Shaohua Wu,Yukun Qin
The Fenton system (Fe2+/H2O2) generates ·OH with a high oxidation potential. However, as reactants themselves, H2O2 and Fe2+ can act as ·OH initiators as well as ·OH scavengers, leading to the need for a high dosage of reactants and increased costs. As a mixing-sensitive reaction, the ·OH-related reaction kinetics (·OH with Fe2+, H2O2, and RhB) was determined from the reaction rates (which were a constant in this work) and stoichiometry, in which the latter could be regulated by an addition strategy of Fenton reagents. This suggests that ·OH competitive reactions could be controlled by applying a macrolevel addition strategy. Herein, the effects of different addition approaches of Fe2+ and H2O2 on ·OH competitive reactions were quantitatively and systematically studied by analyzing the removal of the model pollutant RhB. We found that without stirring, and compared with a one-time addition, once H2O2 or Fe2+ was added in a step-wise pattern (e.g., one drop by one drop, 2 times, or 4 times), a high concentration of H2O2 or Fe2+ existed in a localized place for a longer period, resulting in a lower proportion of ·OH reacting with RhB, which we ascribed to an enhanced reaction between Fe2+, H2O2, and ·OH. However, when H2O2 and Fe2+ were added from two close points without stirring, a larger proportion of ·OH was scavenged by H2O2 and Fe2+; while under stirring, even a one-time addition of H2O2 or Fe2+ could cause severe scavenging of ·OH. The results also revealed a linear relationship between the RhB removal percentage and wavelength blue-shifts. This study showed that microlevel ·OH competitive reactions could be controlled by applying a macrolevel addition strategy of Fenton reagents without the addition of external chemicals. The results suggest this methodology can also offer an approach to lower ·OH invalid consumption by regulating the addition strategy in bigger reactors.
研究领域:
环境化学
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水处理技术
·
高级氧化过程
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反应动力学
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污染控制化学
✓ 已验证
DOI
高影响因子
FUEL
·
2019
·
IF 5.128
Ze Zhang,Jun Cheng,Yi Qiu,Xi Zhang,Junhu Zhou,Kefa Cen
To clarify the conversion mechanism of methyl palmitate (C16:0) to produce jet biofuel over Ni/desilicated meso-Y zeolite catalyst, quantum chemistry calculation and verification experiments were conducted to evaluate three proposed competitive reaction pathways, in which hydrodecarboxylation pathway was more feasible than hydrogenolysis and decarboxylation pathways. It was found that overall enthalpy change to produce pentadecane (−130.2 kJ/mol) in hydrodecarboxylation pathway was lower than that to produce palmitic acid (−90.1 kJ/mol) in hydrogenolysis pathway and that to produce hexadecane (−68.6 kJ/mol) in decarboxylation pathway. The experimental results of hydrodeoxygenation and hydrocracking conversion of methyl palmitate into jet biofuel were consistent with quantum chemistry calculation, when conventional Y zeolite was modified into hierarchical mesoporous Y zeolite catalyst by desilication with NaOH and then loading Ni nanoparticles. The jet biofuel product selectivity reached a peak (64.8%) with reasonable composition distributions, when Ni/meso-Y zeolite was desilicated with 0.4 M NaOH to promote BET surface area (554.9 m 2 /g) and specific pore volume (0.340 cm 3 /g) with 2–10 nm mesopores. The relative content of pentadecane in liquid products was always higher than those of palmitic acid and hexadecane over Ni/meso-Y zeolite catalysts desilicated with various concentrations of NaOH. The main compositions of gas phase by-products in hydrodeoxygenation and hydrocracking conversion were CH 4 with selectivity up to 25.2% and CO 2 with selectivity of ∼10%, which agreed well with quantum chemistry calculation results.
研究领域:
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Laicui Song,Jianlin Li,Hao Li,Yunwei Chang,Shijie Dai,Ruimin Xu,Menghua Dou,Qianjin Li,Guangping lv,Tiesong Zheng
A highly sensitive surface-enhanced Raman spectroscopy (SERS) aptasensor for multiplex mycotoxins detection was developed based on aptamer-functionalized photonic microsphere array. Gold nanoparticles (AuNPs) were grafted covalently onto the silica photonic crystal microsphere (SPCM) to fabricate the SERS active substrate, on which the near-field enhancement can reach to 20 times analyzed by the simulation electric field distribution. Two dyes of 5,5′-dithiobis (2-nitrobenzoic acid) (DTNB) and nile blue A (NBA) were employed to make the SERS nanotags on AuNPs that were modified with corresponding anti-aptamer sequences. A SERS assay system was established based on the competitive reaction between the anti-aptamer on SERS nanotags and the target mycotoxin towards the aptamer on SPCM. The developed method showed a linear relationship in the range of 0.01–100 ng/mL for aflatoxin B 1 (AFB 1 ) and 0.001–10 ng/mL for ochratoxin A (OTA), and a low limit of detection of 0.36 pg/mL for AFB 1 and 0.034 pg/mL for OTA. The accuracy of such method was confirmed by its good recovery ratio and high repeatability, and further verified by the classic enzyme-linked immunosorbent assay using naturally mycotoxins contaminated edible samples. The established method has a great application potential for screening mycotoxins rapidly with high sensitivity, low-cost and high throughput in the fields of food and traditional Chinese herb.
研究领域:
食品科学
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分析化学
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纳米技术
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
研究领域:
环境催化
·
纳米科技
·
可再生能源
·
表面化学
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Yu Fan,Xingrong Tan,Xiaofang Liu,Xin Ou,Shihong Chen,Shaping Wei
A non-enzymatic electrochemiluminescence (ECL) sensor based on the competitive reaction between glucose and phenoxy dextran (DexP) for concanavalin A (ConA) binding sites was constructed for detecting glucose. The hybrid of graphitic carbon nitride nanosheet and 3,4,9,10-perylenetetracarboxylic acid (g-C 3 N 4 -PTCA) as signal probe was modified onto the glass carbon electrode (GCE) for immobilizing DexP through π-π interaction. Then, ConA was incubated onto the electrode via the specific binding between ConA and DexP. When the modified electrode was immersed into glucose solution, glucose would compete with DexP for ConA. With the increase in the concentration of glucose, the more ConA was taken away from the electrode, resulting in a gradual increase in ECL intensity, thus, achieving the determination of glucose. The linear range was 1.0×10 −10 ∼5.2×10 −5 M and the detection limit was 4.0×10 −11 M (S/N = 3). Moreover, this sensor possessed high sensitivity, good stability and reproducibility, indicating a promising development of non-enzymatic ECL glucose sensor.
研究领域:
分析化学
·
生物传感器
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）