POLYMER JOURNAL
·
2023
·Vol. 55
·期 12
·1295-1305
·
IF 2.8
Zhou Qian,Liu Bing,Jia Zhaolei,Gao Xuejiao,Ba Xinwu,Zhang Yuangong,Bai Libin
The aqueous solution of hyperbranched poly(bis-acrylamide)s (HPEAMs) prepared by reversible addition-fragmentation chain transfer (RAFT) polymerization has a lower critical solution temperature (LCST), which can also respond to HCO 3 - . However, the phase change mechanism of HPEAMs has not yet been proven. In this paper, N -(2-propionamidoethyl)acrylamide was designed as a monomer and chain transfer agent (CTA), and the corresponding linear polymers, hyperbranched polymers and hyperbranched copolymers were further prepared. Fourier transform infrared spectroscopy, 1 H nuclear magnetic resonance, ultraviolet‒visible spectroscopy, dynamic light scattering and zeta potential were employed to characterize the structure and phase transition behavior. The results confirmed that the bis-acrylamide unit is hydrophilic and the CTA unit is hydrophobic. The hydrophilic-hydrophobic balance system constructed by the unit of bis-acrylamide and CTA endowed the hyperbranched polybisacrylamide with temperature-responsive behavior, and the carboxyl group in the CTA structural unit is the responsive group that makes it possible to tune the LCST in the presence of HCO 3 - .
研究领域:
高分子化学
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材料科学
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Lixiong Qian,Lei Yao,Yunpeng Liu,Hao Wang,Jiajun Zhong,Chao Liu,Guang Mo,Xueqing Xing,Zhongjun Chen,Zhonghua Wu
The formation mechanism of nanoparticles is of great significance for the controllable synthesis, structural design, and performance optimization of nanomaterials. In this paper, an economical hydrothermal method was used to synthesize zinc oxide (ZnO) nanorods. X-ray diffraction, X-ray absorption fine structure, and small-angle X-ray scattering techniques were used to probe the structural changes. Scanning electron microscopy and high-resolution transmission electron microscopy were used to observe the morphologies of the products. A self-designed in situ temperature–pressure sample cell was used to control the hydrothermal conditions. The results demonstrate that an unknown intermediate phase, Zn(HCO3)2·H2O, was first formed at 50 °C, having a morphology of nanoflakes with a average thickness of about 35 nm. The intermediate phase Zn(HCO3)2·H2O was determined to have a monoclinic structure with space group P1211 and the following lattice parameters: a = 11.567 Å, b = 3.410 Å, c = 5.358 Å, β = 96.0011°, and Z = 2. After a hydrothermal temperature of 140 °C, CO2 and H2O were evaporated from the Zn(HCO3)2·H2O intermediate product and the ZnO nanorods with a wurtzite structure were formed. The final ZnO nanorods have an average diameter of about 45 nm and an average length of about 2 μm. The axial direction of the ZnO nanorods is the [001] crystallographic direction. By virtue of understanding the formation mechanism, this work is helpful for the controllable synthesis of ZnO nanoparticles.
研究领域:
材料科学
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纳米技术
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DOI
PubMed
高影响因子
Science China-Chemistry
·
2024
·
IF 10.4
Wang Yuchen,Shi Wenjie,Tao Weixue,Zhang Jihong,Zhong Di-Chang,Lu Tongbu
Dinuclear metal synergistic catalysis (DMSC) has been evidenced to be effective in enhancing the catalytic activity for CO 2 reduction. However, the reaction kinetics of CO 2 reduction is still limited by the local CO 2 concentration around the dinuclear catalytic centers. Inspired by the structure of carbonic anhydrase, we have designed and synthesized a dinuclear cobalt(II) complex with an –OH group. This complex not only exhibits DMSC for CO 2 reduction but also possesses excellent capture capacity for CO 2 molecules. Consequently, the complex demonstrates high efficiency for the photocatalytic reduction of CO 2 to CO, with turnover number reaching as high as 43,400 and a selectivity of 97%. Even in 10% CO 2 , the complex still shows state-of-the-art catalytic activity. The results of experiments and theoretical calculations reveal that besides the DMSC contributing to the enhanced catalytic activity, the –OH group in the dinuclear cobalt(II) complex facilitates the capture of CO 2 by the formation of HCO 3 − intermediates, thereby enhancing the affinity towards CO 2 and boosting the catalytic activity for CO 2 -to-CO conversion.
研究领域:
化学
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材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 16
·A4014
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IF 3.12
Zhiyuan Song,Xueyu Zhang,Xuesong Li,Lianfeng Duan,Wei Lü
Flexible capacitor systems with high-performance and stretchable characteristics have been widely concerned due to potential applications in portable and wearable electronics. Herein, we prepared PVA/Carbon nanotube (CNT)@Ni(HCO3)2 flexible film as supercapacitor electrodes. CNTs is used as charge transfer pathway to enhance the conductivity of polymer and double-layer capacitance. Ni(HCO3)2 decorated on CNTs provides pseudocapacitance, and PVA matrix provides bendable and stretchable ability. The device achieves a specific capacitance of 143.6 mF cm−2, and the PVA/CNT@Ni(HCO3)2 film exhibits tensile strength of 0.37 MPa with elongation at break of 450%. The flexible device with excellent stretchable and bendable ability shows an instant response to the finger bending with the capacitance change more than 35%, which provides the possibility for fabricating novel smart flexible device to monitor human health and motion detection.
研究领域:
材料科学
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能源存储
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传感器技术
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产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 3
·659
·
IF 4.2
Zedian Li,Liangrui Xiang,Shijia Pan,Dahai Zhu,Shen Li,He Guo
This research constructed a novel O3/CaO2/HCO3−system to degrade antibiotic oxytetracycline (OTC) in water. The results indicated that CaO2andHCO3−addition could promote OTC degradation in an O3system. There is an optimal dosage of CaO2(0.05 g/L) andHCO3−(2.25 mmol/L) that promotes OTC degradation. After 30 min of treatment, approximately 91.5% of the OTC molecules were eliminated in the O3/CaO2/HCO3−system. A higher O3concentration, alkaline condition, and lower OTC concentration were conducive to OTC decomposition. Active substances including ·OH,1O2,·O2−, and ·HCO3−play certain roles in OTC degradation. The production of ·OH followed the order: O3/CaO2/HCO3−> O3/CaO2> O3. Compared to the sole O3system, TOC and COD were easier to remove in the O3/CaO2/HCO3−system. Based on DFT and LC-MS, active species dominant in the degradation pathways of OTC were proposed. Then, an evaluation of the toxic changes in intermediates during OTC degradation was carried out. The feasibility of O3/CaO2/HCO3−for the treatment of other substances, such as bisphenol A, tetracycline, and actual wastewater, was investigated. Finally, the energy efficiency of the O3/CaO2/HCO3−system was calculated and compared with other mainstream processes of OTC degradation. The O3/CaO2/HCO3−system may be considered as an efficient and economical approach for antibiotic destruction.
研究领域:
环境科学
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化学工程
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毒理学
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DOI
PubMed
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
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2024
·Vol. 22
·期 1
·1-13
·
IF 10.6
Yang Peng,Liu Shaojie,Chen Zhuang,Liu Weijing,Duan Deshang,Yang Zuo,Yan Haohao,Rao Zhiping,Zhang Xianghan,Zhang Ruili,Wang Zhongliang
Background Mn 2+ -mediated chemodynamic therapy (CDT) has been emerged as a promising cancer therapeutic modality that relies heavily on HCO 3 − level in the system. Although the physiological buffers (H 2 CO 3 /HCO 3 − ) provide certain amounts of HCO 3 − , the acidity of the tumor microenvironment (TME) would seriously affect the HCO 3 − ionic equilibrium (H 2 CO 3 ⇌ H + + HCO 3 − ). As a result, HCO 3 − level in the tumor region is actually insufficient to support effective Mn 2+ -mediated CDT. Results In this study, a robust nanomodulator MnFe 2 O 4 @ZIF-8 (PrSMZ) with the capability of in situ self-regulation HCO 3 − is presented to enhance therapeutic efficacy of Mn 2+ -mediated CDT. Under an acidic tumor microenvironment, PrSMZ could act as a proton sponge to shift the HCO 3 − ionic equilibrium to the positive direction, significantly boosting the generation of the HCO 3 − . Most importantly, such HCO 3 − supply capacity of PrSMZ could be finely modulated by its ZIF-8 shell thickness, resulting in a 1000-fold increase in reactive oxygen species (ROS) generation. Enhanced ROS-dependent CDT efficacy is further amplified by a glutathione (GSH)-depletion ability and the photothermal effect inherited from the inner core MnFe 2 O 4 of PrSMZ to exert the remarkable antitumor effect on mouse models. Conclusions This work addresses the challenge of insufficient HCO 3 − in the TME for Mn 2+ -mediated Fenton catalysts and could provide a promising strategy for designing high-performance Mn 2+ -mediated CDT agents to treat cancer effectively.
研究领域:
癌症治疗
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纳米技术
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化学生物学
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生物医学工程
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Bo Lv,Xuefan Feng,Xinyan Feng,Xiaoming Wang,Zhenyu Yuan,Bowen Xu,Yu Yang,Fuqin Zhang
Using photocatalysts to produce hydrogen from photocatalytic water splitting is a green approach for producing renewable energy with minimum environmental impact. The key to the success of this technology is to develop an efficient hydrogen production catalyst with stable performance. In this work, we report a simple two-step preparation of zinc carbonate modified with Cd 0.5 Zn 0.5 S/Ni(HCO 3 ) 2 composite. The participation of Ni(HCO 3 ) 2 co-catalyst improved the visible light activity, which also irreversibly inhibited the recombination of holes and electrons. Meanwhile, the novel 0D and 2D heterojunctions are responsible for the excellent catalytic performance with superior stability. The catalytic hydrogen production reached the best rate of 64 mmol/g/h with the cumulative hydrogen production of 320 mmol/g in 5 h, which is even better than that from the photocatalysts activated with the precious metal, Pt. The underlying mechanism was rationalized by the hydrogen evolution kinetics analysis. The excellent hydrogen production performance, presented in this work, demonstrated that the composite of zinc carbonate modified with Cd 0.5 Zn 0.5 S/Ni(HCO 3 ) 2 is a promising, economical and efficient choice of the photocatalyst.
研究领域:
材料科学
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能源化学
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环境科学
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Hang Zhao,Xiuying Liu,Siyu He,Mingxia Guo,Yuhan Huang,Yifan Niu,Haiqing Jiang,Qian Li
Advanced oxidation processes (AOPs) are effective approaches for the removal of organic contaminants from water. In this study, a combined hydrogen peroxide-bicarbonate (H 2 O 2 -HCO 3 − ) oxidant system was engineered for a Fenton-like process catalyzed by lithium cobalt oxide (LCO). The oxidant system integrates hydrogen peroxide oxidation with bicarbonate's dual functionality as both an H 2 O 2 activator and pH buffer. Efficient contaminant degradation was achieved by the LCO/H 2 O 2 HCO 3 − system under neutral or weakly alkaline conditions, and the solution pH remained stable throughout the reaction, due to the presence of HCO 3 − . A comprehensive investigation into the optimization of reaction parameters governing the removal of a phenothiazine dye was conducted. The mechanism driving the generation of reactive oxygen species (ROS) which are responsible for the degradation of organic contaminants was elucidated. These ROS were identified as superoxide radicals, singlet oxygen, and hydroxyl radicals. The Co(III)/Co(II) redox pair in LCO served as the key active sites for activating the H 2 O 2 HCO 3 − . In addition, a possible pathway of the degradation of the phenothiazine structure was proposed based on ultraviolet-visible spectroscopy and liquid chromatography-mass spectrometry analysis. The LCO/H 2 O 2 -HCO 3 − system shows great promise as a sustainable Fenton-like approach for wastewater treatment, with cost-effectiveness, high efficiency, environmental friendliness, and compatibility with neutral or weakly alkaline conditions.
研究领域:
环境化学
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材料科学
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水处理技术
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催化
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2020
·
IF 4.825
Zi-He Meng,Song-Hai Wu,Shi-Wei Sun,Zhi Xu,Xiao-Cong Zhang,Xiang-Ming Wang,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,He Bai,Xu Han
The MnII(HCO3–)–H2O2 (MnII-BAP) system shows high reactivity toward oxidation of electron-rich organic substrates; however, the predominant oxidizing species and its formation pathways involved in the MnII-BAP system are still under debate. In this study, we used the MnII-BAP system to oxidize As(III) in that As(III), Mn2+, and HCO3– are common components in As(III)-contaminated groundwater. Kinetic results show that MnII(HCO3–)n [including MnII(HCO3)+ and MnII(HCO3)2] is a key factor in the MnII-BAP system to oxidize As(III). Quenching experiments rule out contributions of OH• and 1O2 to As(III) oxidation and reveal that O2•– and the oxidizing species generated from O2•– play predominant roles in the oxidation of As(III). We further reveal that the MnO2+(HCO3–)n intermediate generated in the reaction between MnII(HCO3–)n and O2•–, instead of O2•–, is the predominant oxidizing species. Although CO3•– also contributes to As(III) oxidation, the high reaction rate constant between CO3•– and O2•– indicates that CO3•– is not the predominant oxidizing species in the As(III)-MnII-BAP system. In addition, the presence of Mn(III) further indicates the important Mn(II)–Mn(III) cycling in the MnII-BAP system. We therefore suggest two important roles of MnII(HCO3–)n in the MnII-BAP system: (i) MnII(HCO3–)n reacts with H2O2 to form the MnIII(HCO3)3 intermediate, followed by a subsequent reaction between MnIII(HCO3)3 and H2O2 to produce O2•–; (ii) MnII(HCO3–)n can also stabilize O2•– with the formation of MnO2+(HCO3–)n. MnO2+(HCO3–)n is an electrophilic reagent and plays the predominant role in the oxidation of As(III) to As(V).
研究领域:
环境化学
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水处理
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氧化还原化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Mingmin Jia,Xiong-Fei Zhang,Yicheng Zhou,Hengyang Mao,Yijiang Zhao,Jianfeng Yao
In this work, Amine-functionalized CNF/UiO-66 (CNF–NH 2 /UiO-66) composite membranes were fabricated by incorporating UiO-66 nanoparticles in the CNF–NH 2 matrix. The CO 2 -facilitated transfer channels can be constructed in the CNF–NH 2 /UiO-66 composite membrane. As a natural polymer material, CNF–NH 2 would absorb water and form a gel-like structure under humidification. The adsorbed water can convert CO 2 into bicarbonate ions (HCO 3 − ) through the catalysis of amino groups on CNF–NH 2 . Moreover, in CNF–NH 2 /UiO-66 composite membranes, HCO 3 − could quickly migrate to the permeate side promoted by the porous UiO-66, facilitating CO 2 transport. The optimum membrane gave a CO 2 permeability of 257.0 Barrer with a CO 2 /CH 4 ideal selectivity of 71.3.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2025
·Vol. 26
·期 2
·677
·
IF 4.9
Yuhan Zhang,Guilong Peng,Yuting Yan,Xukun Meng,Wenwen Gong
The design of efficient advanced oxidation processes (AOPs) in the presence of bicarbonate has long attracted considerable attention in the field of environmental catalysis. In this study, sodium bicarbonate (NaHCO3) as one of the most abundant substances in actual water, was introduced to a NaClO/Ru(III) system to enhance the removal of acid orange 7(AO7). NaHCO3could significantly improve the removal efficiency of the Ru(III)/NaClO process in HCO3−at a pH range of 6.9–10.0. Ru(V)=O was identified as a dominant reactive species involved in the degradation of pollutants in the NaHCO3/NaClO/Ru(III) system. HCO3−interacts with Ru(III) to generate Ru(III)-HCO3−, which enhances the activation performance of Ru(III) under neutral or alkaline conditions. The removal of AO7 was significantly enhanced with increasing NaHCO3concentration, and the rate constant increased more than 2-fold to 4-fold as NaHCO3concentrations increased from 0 to 100 mM at pH 6.9 and 8.5. This study proposed a novel strategy to enhance the Ru(III)/NaClO process with environmentally friendly inorganic ligands and highlights its potential applications in the removal of pollutants.
研究领域:
环境催化
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化学工程
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水处理技术
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产品关联
DOI
PubMed
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2021
·
IF 6.291
Yimin Zhang,Jingkun Lou,Leliang Wu,Minghua Nie,Caixia Yan,Mingjun Ding,Peng Wang,Hua Zhang
Homogeneous Cu 2+ -mediated activation of H 2 O 2 has been widely applied for the removal of organic contaminants, but fairly high dosage of Cu 2+ is generally required and may cause secondary pollution. In the present study, minute Cu 2+ (2.5 μM) catalyzed H 2 O 2 exhibited excellent efficiency in degradation of organic pollutants with the assistant of naturally occurring level HCO 3 − (1 mM). In a typical case, acetaminophen (ACE) was completely eliminated within 10 min which followed the pseudo-first-order kinetics. Singlet oxygen and superoxide radical rather than traditionally identified hydroxyl radical were the predominant reactive oxygen species (ROS) responsible for ACE degradation. Meanwhile, Cu 3+ was deduced through Cu + and p -hydroxybenzoic acid formation analysis. CuCO 3 (aq) was the main complex with high reactivity for the activation of H 2 O 2 to form ROS and Cu 3+ . The removal efficiency of ACE depended on the operating parameters, such as Cu 2+ , HCO 3 − and H 2 O 2 dosage, solution initial pH. The presence of Cl − , HPO 4 2− , humic acid were found to retard ACE removal while other anions such as SO 4 2− and NO 3 − had no obvious effect. ACE exhibited lower degradation efficiency in real water matrices than that in ultra-pure water. Nevertheless, 58–100% of ACE was removed from domestic wastewater, lake water and tap water within 60 min. Moreover, eight intermediate products were identified and the possible degradation pathways of ACE were proposed. Additionally, other typical organic pollutants including bisphenol A, norfloxacin, lomefloxacin hydrochloride and sulfadiazine, exhibited great removal efficiency in the Cu 2+ /H 2 O 2 /HCO 3 − system.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子