Nature Communications
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2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Chen Jiadong,Chen Chunhong,Qin Minkai,Li Ben,Lin Binbin,Mao Qing,Yang Hongbin,Liu Bin,Wang Yong
Noble metal electrocatalysts (e.g., Pt, Ru, etc.) suffer from sluggish kinetics of water dissociation for the electrochemical reduction of water to molecular hydrogen in alkaline and neutral pH environments. Herein, we found that an integration of Ru nanoparticles (NPs) on oxygen-deficient WO 3-x manifested a 24.0-fold increase in hydrogen evolution reaction (HER) activity compared with commercial Ru/C electrocatalyst in neutral electrolyte. Oxygen-deficient WO 3-x is shown to possess large capacity for storing protons, which could be transferred to the Ru NPs under cathodic potential. This significantly increases the hydrogen coverage on the surface of Ru NPs in HER and thus changes the rate-determining step of HER on Ru from water dissociation to hydrogen recombination.
研究领域:
电化学
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材料科学
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催化
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能源材料
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
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IF 8.8
Dingxi Zhang,Yuping Xiang,Guangliang Liu,Lina Liang,Lufeng Chen,Jianbo Shi,Yongguang Yin,Yong Cai,Guibin Jiang
Methylmercury (MeHg), derived from industrial processes and microbial methylation , is still a worldwide environmental concern. A rapid and efficient strategy is necessary for MeHg degradation in waste and environmental waters. Here, we provide a new method with ligand-enhanced Fenton-like reaction to rapidly degrade MeHg under neutral pH. Three common chelating ligands were selected (nitriloacetic acid (NTA), citrate, and ethylenediaminetetraacetic disodium (EDTA)) to promote the Fenton-like reaction and degradation of MeHg. Results showed that MeHg can be rapidly degraded, with the following efficiency sequence: EDTA > NTA > citrate. Scavenger addition demonstrated that hydroxyl radical ( ▪ OH), superoxide radical (O 2 ▪– ), and ferryl (Fe Ⅳ O 2+ ) were involved in MeHg degradation, and their relative contributions highly depended on ligand type. Degradation product and total Hg analysis suggested that Hg(Ⅱ) and Hg 0 were generated with the demethylation of MeHg. Further, environmental factors, including initial pH, organic complexation (natural organic matter and cysteine), and inorganic ions (chloride and bicarbonate) on MeHg degradation, were investigated in NTA-enhanced system. Finally, rapid MeHg degradation was validated for MeHg-spiked waste and environmental waters. This study provided a simple and efficient strategy for MeHg remediation in contaminated waters , which is also helpful for understanding its degradation in the natural environment.
研究领域:
环境科学
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毒理学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2018
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IF 3.927
Pan Gao,Yuan Song,Mengjie Hao,Anna Zhu,Hongwei Yang,Shaoxia Yang
A novel Fe 2 O 3 -ZrO 2 catalyst was prepared by the sol-gel method, and investigated for phenol degradation in the Fenton-like reaction under neutral pH condition. The ZrO 2 addition increased the surface areas of the catalyst. Scanning electron microscopy (SEM) showed that ZrO 2 nano-particle dispersed on the surface of Fe 2 O 3 . X-ray photoelectron spectroscopy (XPS) indicated that the Fe 2+ amount increased with the increase of the Zr content on the surface. The Fe 2 O 3 -ZrO 2 catalyst produced hydroxyl radicals (OH ) and superoxide radicals (O 2 − /HO 2 ), and exhibited good catalytic performance in the reaction. Total phenol conversion and 56% TOC removal were achieved after 210 min under neutral pH at 60 °C in the heterogeneous Fenton-like reaction. In addition, the prepared Fe 2 O 3 -ZrO 2 catalyst had good magnetism.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
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2021
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IF 9.676
Pan Sun,Yahua Liu,Peipei Zuo,Yuanyuan Li,Qianru Chen,Zhengjin Yang,Tongwen Xu
Aqueous flow batteries (AFBs) are among the most promising electrochemical energy storage solutions for the massive-scale adoption of renewable electricity because of decoupled energy and power, design flexibility, improved safety and low cost. The development of high-voltage AFB is, however, limited by the lack of stable anolytes that have low redox potential. Here we report Eu-based anolytes for high-voltage pH-neutral AFB applications. Eu 3+ has a reduction potential of −0.39 V vs. SHE, which can be dramatically lowered when forming stable complex with inexpensive organic chelates. A typical complex, EuDTPA, features a low redox potential of −1.09 V vs. SHE, fast redox kinetics, and a high water solubility of 1.5 M. When paired with ferrocyanide, the battery had an open-circuit voltage of 1.56 V and demonstrated stable cell cycling performance, including a capacity retention rate of 99.997% per cycle over 500 cycles at 40 mA cm −2 , a current efficiency of >99.9%, and an energy efficiency of >83.3%. A high concentration anolyte at 1.5 M exhibited a volumetric capacity of 40.2 Ah L −1 , which is one of the highest known for pH-neutral AFBs, promising a potent solution for the grid-scale storage of renewable electricity.
研究领域:
能源化学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhiyu Wei,Xiaoqin Li,Shuang Han,Cihang Yan,Mingchao Sun,Yong Liu,Lu Fan
To expand the working pH range of NO 3 – -N reduction from aqueous solution, a two-step method including the Al/Cu bimetal and sulfamic acid reduction was developed. In this process, Al/Cu bimetallic materials were prepared by chemical deposition method and characterized by EDS, SEM, XRD and XPS. The NO 3 – -N reduction batch experiment showed that 100% of NO 3 – -N was reduced and converted to N 2 at pH of 7, Al/Cu dosage of 30 g/L and EDTA-2Na concentration of 6 mmol/L. When the pH value was adjusted to 3, 5 and 9, NO 3 – -N reduction efficiencies ca. 80–97% were also obtained in the first step, and 100% N 2 selectivity was further obtained with the second reduction step at pH of 3, 7 and 9. The kinetics study indicated that the Al/Cu reduction process was in accordance with the pseudo-second order kinetics model.
研究领域:
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
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 31
·47549-47560
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IF 5.19
You Wenqiao,Li Youlin,He Dandan,Zeng Youmei,Zhu Jiangwei,You Xiaofeng,Wang Kang,Zhou Guangming,Peng Guilong
In the present study, pyrophosphate (PP) was used to activate peroxymonosulfate (PMS) for acid orange 7 (AO7) removal under neutral pH conditions. The removal rate of AO7 (20 mg/L) was 84% within the reaction time with a rate constant value of 0.0165 min −1 under optimum conditions. Additionally, the effects of the concentrations of PMS and PP in solutions with various pH values and the coexisting inorganic anions on AO7 removal were measured. In addition, the performance of phosphate (P(V)) on PMS activation was compared with that of phosphite (P(III)) species. In contrast to P(III), the concentration of P(V) showed a positive correlation with the efficiency of AO7 decolorization. PMS activation in different types of buffer solutions was also examined, and the results indicated that the decolorization efficiency of AO7 induced by PP addition, and the buffer solution also contributed to PMS self-decomposition. Singlet oxygen ( 1 O 2 ) might be the primary reactive oxygen species (ROS) in the PP/PMS system in which AO7 is decolorized at an initial pH of 7.06, as indicated by quenching experiments and electron spin resonance (ESR) tests. Therefore, PP/PMS systems may be promising technologies for removing organic contaminants, particularly for PP-rich electroplating wastewater.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
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2012
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IF 4.186
Zan Zhao,Liang Yin,Gang Yuan,Liyan Wang
We fabricated a layer-by-layer (LbL) film of temperature-responsive homopolymers at neutral pH and studied its temperature-dependent solubility. We first measured the cloud point of mixed solutions of temperature-responsive polymers. The significant decrease of cloud point suggested that the intermolecular interaction between two polymer chains of different kinds was stronger than that between two polymer chains of the same kind. Strong intermolecular interaction between two polymer chains of different kinds is a prerequisite for LbL assembly. On the basis of the decrease of cloud point of mixed solutions of temperature-responsive homopolymers, we selected poly(N-vinylcaprolactam) (PVCL) and poly(2-hydroxypropyl acrylate) (PHPA) for LbL assembly. LbL films of the two polymers were fabricated at neutral pH at a constant temperature. When the film was immersed in purified water at a temperature lower than the assembly temperature, it can be partially dissolved with a diffusion-limited dissolution process. The temperature-responsive solubility of the LbL film is closely connected to the phase behavior of mixed solutions of the two polymers. Additionally, as compared to multilayer films of neutral polymers and poly(carboxylic acid)s, the PVCL/PHPA multilayer film is relatively stable when it was immersed in buffer solutions near physiological pH at the assembly temperature. Such LbL films with temperature-responsive solubility might be used as a dissolvable film or a smart capsule.
研究领域:
材料科学
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高分子化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Xiaotong Chen,Qiaohan Li,Huiqiang Li,Ping Yang,Zilong Zou
A novel nickel foam (NF) supported core–shell catalytic material with excellent catalytic performance was successfully prepared for the degradation of salicylic acid (SA) by heterogeneous electro-Fenton (HEEF). Under the reaction conditions of SA initial concentration of 100 mg/L, catalyst dosage of 4 g/L, aeration rate of 0.1 L/min, current of 0.3 A and pH of 7, after 2 h, the removal efficiency of the progressively modified core–shell catalysts for SA and COD was as follows: NF@Fe 3 O 4 @SiO 2 @MgAl-LDH > NF@Fe 3 O 4 @MgAl-LDH > NF@Fe 3 O 4 > NF@Fe 3 O 4 @SiO 2 . The removal efficiency of NF@Fe 3 O 4 @SiO 2 @MgAl-LDH for SA and COD reached 72.8 % and 52.12 %, respectively. The morphology, composition and structural characteristics of the composite catalysts were analyzed and compared by a series of characterization methods. Among them, NF@Fe 3 O 4 @SiO 2 @MgAl-LDH showed the largest Fe:Ni atomic content ratio, specific surface area and pore volume, with values of 1: 2.62, 7.5405 m 2 ·g −1 and 0.010504 cm 3 ·g −1 , respectively. Radical quenching experiments, changes in H 2 O 2 and Fe 2+ ion concentrations, and X-ray photoelectron spectroscopy (XPS) analysis revealed the reaction mechanism of the HEEF process. That is, synergistic oxidation of active radicals and abundant adsorbed oxygen and lattice oxygen on the surface of the materials promoted the degradation and mineralization of SA. The excellent stability and reusability of NF@Fe 3 O 4 @SiO 2 @MgAl-LDH in the HEEF system were verified through five cyclic experiments with low material loss rate and sludge production.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yu Chen,Yajing Li,Yongjian Wang,Igor Ying Zhang,Rongfu Huang
This work investigated the activation of peroxymonosulfate by electrochemical (EC) system assisted with Fe(III)-nitrilotriacetic acid (NTA) complex for degradation of persistent naphthenic acids (NAs) under neutral initial pH conditions. As NAs are a complicated mixture, 1-adamantanecarboxylic acid (ACA) was selected as the model NA compound for degradation experiment. The addition of NTA is to chelate with Fe(III), gaining stability under neutral pH condition to facilitate the circulation of Fe(II)/Fe(III) by the electrochemical process to activate PMS. The EC/Fe(III)-NTA/PMS system was explored with applicable pH range of 3–9 and an optimized molar ratio 1: 2 for Fe: NTA. Results of quenching and chemical probe experiment together with results of electron paramagnetic resonance (EPR) analysis revealed the main reactive species of the system, including • OH, SO 4 •− , 1 O 2 and possibly Fe(IV). With the addition of NTA, the yields of • OH, SO 4 •− , 1 O 2 were enhanced. Results of mass spectrometry analysis and DFT calculations indicated the formation of 9 degradation byproducts of ACA via three primary degradation pathways such as hydroxyl substitution, carbonyl substitution, and decarboxylation . Furthermore, the EC/Fe(III)-NTA/PMS system could achieve excellent removal efficiency of ACA with different anions such as Cl - , HCO 3 - , NO 3 - and H 2 PO 4 - in the background. The practical applicability of the system was also verified with the high removal of commercial NAs mixture standard. Overall results have indicated the EC/Fe(III)-NTA/PMS system could be utilized for efficient reclamation of authentic oil and gas industrial wastewater under natural pH conditions.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Xuechao Xu,Juanli Yang,Qiao Guo,Lu Gao,Bo Wang,Suhui Tan,Kun Wang,Yun-xia Li,Shengyan Zhao,Yi Li,Zhen-quan Yang
Reassessment of total antioxidant capacity (TAC) in Cordyceps militaris is imperative for providing dietary guidance and facilitating health monitoring. Herein, surface-carboxylated cobaltous oxide (COOH-Co 3 O 4 ) nanozyme was achieved via a dual-stage procedure encompassing reduction preparation and surface modification. COOH-Co 3 O 4 exhibited exceptional oxidase-like activity under neutral pH conditions, facilitating conversion of dissolved oxygen into superoxide anion free radicals and subsequently catalyzing oxidation of colorless 3, 3′, 5, 5′-tetramethylbenzidine (TMB) to yield blue oxidized TMB (TMBox) at neutral pH. Additionally, antioxidants can eliminate O 2 · − produced in the above reaction system. Moreover, the absorbance at 652 nm of the COOH-Co 3 O 4 + TMB reaction system gradually diminishes with an increase in ascorbic acid concentration. Based on it, a colorimetric evaluation system (using ascorbic acid as a reference) for TAC of C. militaris was established. This innovative approach offers an impressively low limitation of detection (LOD) calculated as 0.78 μM. Furthermore, it was employed to evaluate TAC of real C. militaris samples, yielding a satisfactory recovery (96.1 %–102.3 %), thereby demonstrating its exceptional accuracy. The TAC of C. militaris extracted using different solvents was determined, indicating that the highest TAC is observed in C. militaris extracted by deionized water. This study not only offers a rapid, cost-effective, and convenient analytical tool for evaluating TAC of C. militaris but also expands the potential applications of nanozymes.
研究领域:
食品科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Ge Song,Yang Zheng,Minghua Zhou
The application of bimetallic catalysts in heterogeneous electro-Fenton (Hetero-EF) is limited due to its poor performance over a wide pH range. In this work, the Hetero-EF/sulfite process was constructed with FeMn@C as the catalyst to improve the degradation of pollutants under neutral pH. The removal efficiency of diclofenac (DCF) (97.8%) was significantly higher than that of Hetero-EF (15.0%) at pH 7, in which the degradation rate constant k was increased by 19.75 times. The existence and transformation process of various active species ( • OH, SO 4 •- , O 2 •- , and 1 O 2 ) in the process were verified by capture experiments and electron paramagnetic resonance (EPR) test. The possible DCF degradation pathway was also proposed. The introduction of sulfite could reduce Fe 3+ and Mn 3+ , promote the Fe(II)/Fe(III) and Mn(II)/Mn(III) cycles, strengthen the generation of active species, and thus promote the degradation of pollutants. The removal efficiency was still maintained 76.6% after five cycles. The Hetero-EF/sulfite process is a simple, feasible, and efficient method to degrade pollutants, which has a broad application prospect.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhao Yang,Yong Liu,Jianlong Wang
Zero-valent copper (ZVC) has shown potential as an oxygen activator for the degradation of organic pollutants from aqueous solution. Nevertheless, the high leaching of copper ions and the demand for acidic condition limited its application. In this study, a novel mesoporous carbon hybrid loaded zero-valent copper (Cu 0 /C) was successfully synthesized from Cu-based metal–organic framework (Cu 3 (BTC) 2 ) through a pyrolysis method and applied to efficiently degrade sulfamethazine (SMT) at neutral pH under aeration condition. The performance of Cu 0 /C composite for the activation of molecular oxygen was evaluated based on the effect of different reaction parameters, such as, initial SMT concentration, initial pH, activator dosage and reaction temperature. The results showed a high efficiency for SMT removal over a broad pH range (3.0–7.0). Moreover, the Cu 0 /C composite exhibited excellent stability and reusability for SMT degradation, and a 96.7% SMT removal and a 68.8% total organic carbon (TOC) conversion were achieved at pH 5.8 after continuous three cycles. Combined with the determination results of reactive oxidizing species and physical-chemical characterization, cupryl species (Cu 3+ ) rather than OH produced by the reaction of the in-situ generated H 2 O 2 with Cu + were the major reactive species. Additionally, the possible reaction mechanism of Cu 0 /C activated oxygen was tentatively proposed.
研究领域:
环境科学
·
材料化学
✓ 已验证
DOI
高影响因子
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