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).
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高影响因子
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 - .
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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.
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JOURNAL OF NANOBIOTECHNOLOGY
·
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.
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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.
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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.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Te Tu,Jiaqi Zhang,Mengni Xiao,Feihong Liang,Enyu Wang,Lanlan Wu,Long Ji,Shuiping Yan
A novel strategy is proposed to lower CO 2 regeneration energy in DAC. • Monovalent-selective AEMs capable of selectively separating HCO 3 − and CO 3 2− were prepared. • The optimized membrane exhibited a superior HCO 3 − /CO 3 2− perm-selectivity of 24.2. • Specific energy consumption for CO 2 regeneration was reduced by 59.3% compared to commercial AEMs. • The fabricated AEMs exhibited both high HCO 3 − /CO 3 2− perm-selectivity and total carbon permeability. Direct air capture (DAC) is an emerging technology for reducing atmospheric CO 2 content directly, but its current deployment is limited by the high energy demand in CO 2 regeneration. As an energy-conserving alternative, bipolar membrane electrodialysis (BPMED) exploits pH differentials to drive CO 2 regeneration without external thermal inputs or pressurized environments. In this work, we propose a new strategy to construct anion exchange membranes (AEMs) with high carbon loading capacity, enabling preferential permeation of bicarbonate (HCO 3 − ) over carbonate (CO 3 2− ) to significantly reduce specific electrical energy consumption for CO 2 regeneration in BPMED. AEMs were synthesized in a single-casting-process fabrication that integrates the dual advantages of electrostatic regulation and self-crosslinking, achieved through the incorporation of trimethylamine and sulfamerazine (SF) into 2,6-dimethyl-1,4-phenylene oxide (BPPO). The resulting membranes exhibited low water uptake (<12.6%), minimal linear expansion rate (<3.5%), and an area resistance as low as 2.7 Ω cm 2 . The perm-selectivity ( P CO 3 2 ‐ HCO 3 ‐ ) declined with increasing applied current density. At 5 mA/cm 2 current density, the optimized AEM (BPPO-SF-0.12) exhibited a HCO 3 − permeability of 0.21 mmol/(cm 2 ·h) and a CO 3 2− permeability of 0.04 mmol/(cm 2 ·h), yielding a perm-selectivity value of 24.2, substantially higher than that of the commercial membrane (1.0). In BPMED-based CO 2 regeneration, BPPO-SF-0.12 achieved the highest CO 2 regeneration ratio of 45.3%, and its energy consumption was only 240 kJ/mol, corresponding to a 59.3% reduction relative to the commercial membrane (590 kJ/mol). These findings substantiate the efficacy of the proposed strategy, revealing that AEMs with elevated carbon loading concurrently augment CO 2 regeneration ratio and energy performance. Such results establish a practical framework for energy-minimal CO 2 liberation via BPMED technology. Download: Download high-res image (318KB) Download: Download full-size image
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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.
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高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Zhiyan Hou,He Meng,Xueqing Shao,Xianglong Wang,M. Usman Tahir,Shakiaz Ahmad,Chao Yang,Xintai Su,Lijuan Zhang
The complex composition and recycling process of electroplating sludge are the two major obstacles restricting the recycling of metal resources. In this work, Ni(HCO 3 ) 2 hollow spheres with unique amorphous structure were prepared via a simple and controllable hydrothermal method using nickel-containing electroplating sludge as raw material and ascorbic acid (AA) as complexing agent . The introduction of AA not only changed the morphology of the sample, but also formed pure phase Ni(HCO 3 ) 2 . The controllable amorphous structure is beneficial to the diffusion of OH - in the electrolyte. More importantly, its disordered atomic arrangement and metastable structure provide a large number of active sites and ion transmission channels, which improve the specific capacity. Consequently, amorphous Ni(HCO 3 ) 2 delivers a large capacitance of 599.8 C g −1 at 1 A g −1 , besides large capacitance, it also exhibits large rate capability (61.02% at a current density of 10 A g −1 ) and cycle performance (capacitance retention 52.09% after 1000 cycles). Importantly, the recoveries of nickel, iron and aluminum are 95.57%, 99.92% and 92.30%, respectively, indicating that electroplating sludge has a good application prospect as electrode materials for supercapacitors .
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ACS Applied Nano Materials
·
2020
·
IF 0
Qingnan Wu,Ming Wen,Weixi Yan,Qingsheng Wu,Hezhong Wang,Yongqing Fu
A functionalized carbon nanotube (FCNT)/Ni(HCO3)2-Ni nanostructures were synthesized by decorating nanoflaky and mesoporous Ni(HCO3)2 onto FCNT along with in situ formed reduced metallic Ni for the purpose of constructing an energy-storage system with both high specific capacity and cycling stability. Such flaky nanostructures can significantly increase the contact surface areas between the mesoporous and nanoflaky Ni(HCO3)2-Ni and electrolyte, thus immensely reducing the electrolyte-ion diffusion paths and accelerating the electron-transport rates through the use of a FCNT. The in situ reduced metallic Ni atoms are directly contacted with the electrolytes and quickly converted into NiOOH in the alkaline environment. For this reason, the capacity retention of battery-type electrochemical materials can be significantly enhanced, especially at the beginning of cycles. The obtained flaky FCNT/Ni(HCO3)2-Ni nanomaterials exhibit excellent electrochemical performances with a high specific capacity of 203 mAh·g–1 at 3 A·g–1 current density for supercapacitor energy-storage systems. An aqueous asymmetric supercapacitor made of FCNT/Ni(HCO3)2-Ni//graphene oxide achieves a 132 Wh·kg–1 energy density at 2880 W·kg–1 power density and an excellent cycling stability with 84% after 6000 cycles.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 16
·5315-5326
·
IF 4.052
Shaolei Zhao,Keyu Tao,Yun Gong
Co-Incorporated NiV2O6/Ni(HCO3)2 arrays with different morphologies can grow on nickel foam (NF) via a mild one-step hydrothermal method. Among them, S-0.5-20 and S-0.25-20 were obtained at a 1 : 1 : 20 molar ratio of Co/V/urea with 0.5 and 0.25 mmol Co(NO3)2, respectively. They demonstrate high areal capacities of 0.99 mA h cm−2 (7.94 F cm−2) and 0.56 mA h cm−2 (4.48 F cm−2) at 1 mA cm−2, respectively, which are superior to that of Co-incorporated Ni(HCO3)2/NF synthesized in the absence of Na3VO4. S-0.25-20 possesses good rate capability with 82.1% retention when the current density is increased 20-fold, and it shows superior long-term durability with 106.2% retention of the initial capacity after 10 000 charging/discharging cycles at 100 mA cm−2. These results are associated with the porous and orderly hierarchical Co-incorporated NiV2O6/Ni(HCO3)2 nanoflake arrays directly grown on the Ni foam. Moreover, due to the synergetic effect of the individual components, electrons can be transferred from V centers to Ni active sites, thus improving the stability of the vanadate. The generation of more active species, such as Co3+, during cycling could account for the increased capacity. A S-0.25-10//activated carbon (AC) asymmetrical supercapacitor shows a high energy density of 0.533 mW h cm−2 at a power density of 0.232 mW cm−2 (0.415 mW h cm−2 at 4.983 mW cm−2). Furthermore, the formation mechanism of the Co-incorporated NiV2O6/Ni(HCO3)2 nanoflake arrays is proposed.
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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.
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