CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zizheng Liu,Jiawei Liu,Haike Yang,Jingyi Guo,Yiqun Chen,Qing Shao,Shuxian Gao,Liting Luo
Arsenic is categorized as a class I carcinogen due to its strong biological toxicity. In this study, a novel treatment process with Cu 2 (OH) 2 CO 3 as catalyst is proposed, whereby As(III) in water is oxidized by activating sulfite to generate SO 4 − and SO 5 − radicals. Under conditions of [Cu 2 (OH) 2 CO 3 ] 0 = 0.01 g·L −1 , [sulfite] 0 = 0.3 mmol·L −1 , and initial pH 8.0, 94% of As(III) was converted into As(V) within 20 min, whereby dissolved oxygen had a pivotal impact on the reaction. However, HCO 3 − , humic acid, and fulvic acid all significantly inhibited the oxidation. Heterogeneous electron transfer on the catalyst surface and homogeneous dissolved Cu 2+ jointly activated sulfite in the Cu 2 (OH) 2 CO 3 /sulfite system, with the heterogeneous process predominating. Density functional theory (DFT) calculations disclose a dominate physical adsorption of sulfite on Cu 2 (OH) 2 CO 3 surface with 1.74 electrons transferred. >90% of As(III) was still oxidized after recycling the material five times, indicating excellent reusability. Overall, it shows good potential for application in the removal of As(III) from real water samples.
研究领域:
环境科学
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化学
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DOI
高影响因子
DESALINATION
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2025
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IF 9.8
Tianshu Bao,Chenye Wang,Huiquan Li,Liangbin Li,Zhenhua Sun,Yong Wang,Xinjuan Hou,Aiping Peng,Ming Ye
The growing demand for lithium in the new sustainable society is advancing technology for lithium recycling from real Salt Lake brine, which has low concentrations in a near-neutral condition. Traditional adsorbents for this process typically exhibit excellent adsorption ability in alkaline solutions, limiting their industrial application for recycling lithium from the real salt lake. In this work, we designed and synthesized a manganese-based ion sieve loaded onto a cross-linked polystyrene carrier and modified it, HMO@PS-IDA, by incorporating iminodiacetate onto a polystyrene-based ion sieve. These conditions typically reduce the charge density on the surface of adsorbents, hindering the ion exchange process. Our innovative approach introduces cross-linked polystyrene for adsorbent granulation, providing modification sites, and selects Iminodiacetic acid (IDA) as the preferred anionic donor. The dual-structure design of anionic groups and ion sieves in HMO@PS-IDA results in a remarkable 2.6-fold increase in adsorption capacity at pH = 7, surpassing the individual capacities of its components. The adsorbent exhibits a regular spherical shape with a rough surface and uniformly distributed ion sieves, achieving an adsorption capacity of 6.85 mg·g −1 within 40 min in a real neutral system. The synergistic adsorption mechanism is attributed to the CHELPG atomic charge decrease from −0.16 to −1.44, maintaining the ion exchange driving force under neutral conditions. This innovation compensates for the loss of surface charge on the adsorbent, enabling a wide pH application range and overcoming the low adsorption capacity issue in near-neutral conditions. HMO@PS-IDA also demonstrates exceptional lithium adsorption capacity, with a 10-cycle adsorption capacity of 6.3 mg·g −1 , maintaining 92.1 % of the initial performance. These properties make HMO@PS-IDA a direct candidate for extracting Li + from neutral salt lake brines, and our findings provide a theoretical foundation for the modification of adsorption materials.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 10
·2195
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IF 3.1
Yu Liu,Panpan Li,Zegao Wang,Liangjuan Gao
This study reported a multi–functional Co0.45Fe0.45Ni0.9–MOF/NF catalyst for oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and overall water splitting, which was synthesized via a novel shape–preserving two–step hydrothermal method. The resulting bowknot flake structure on NF enhanced the exposure of active sites, fostering a superior electrocatalytic surface, and the synergistic effect between Co, Fe, and Ni enhanced the catalytic activity of the active site. In an alkaline environment, the catalyst exhibited impressive overpotentials of 244 mV and 287 mV at current densities of 50 mA cm−2and 100 mA cm−2, respectively. Transitioning to a neutral environment, an overpotential of 505 mV at a current density of 10 mA cm−2was achieved with the same catalyst, showing a superior property compared to similar catalysts. Furthermore, it was demonstrated that Co0.45Fe0.45Ni0.9–MOF/NF shows versatility as a bifunctional catalyst, excelling in both OER and HER, as well as overall water splitting. The innovative shape–preserving synthesis method presented in this study offers a facile method to develop an efficient electrocatalyst for OER under both alkaline and neutral conditions, which makes it a promising catalyst for hydrogen production by water splitting.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
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2025
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IF 6.1
Mao Huang,Rui Wang,Fan Yu,Qi Ding,Yanyan Zhu
Tanshinol, an active ingredient extracted from the Salvia miltiorrhiza herb, is widely used in Chinese medicine or health supplements. Accurately and rapidly quantifying of tanshinol under near-neutral or neutral conditions is of great significance but still a significant challenge. Herein, a novel electrochemical sensor based on bimetallic FeCo phosphides (Fe x Co 1-x P) was developed for rapid and sensitive detection of tanshinol in near-neutral environments. Fe x Co 1-x P nanocrystals supported on porous graphene (Fe x Co 1-x P/GFs) were synthesized, with Fe 0.25 Co 0.75 P/GFs demonstrating an enhanced electrochemical response for tanshinol detection at pH 6.5. The Fe 0.25 Co 0.75 P/GFs-based tanshinol electrochemical sensor exhibited linear detection ranges of 0.20–11.65 μM and 11.65–39.98 μM, which could accurately quantify tanshinol in Salvia miltiorrhiza herb. This study highlights the potential of earth‐abundant FeCo phosphides for the electrochemical detection of tanshinol under benign conditions, offering a promising approach for the standardized analysis of Salvia miltiorrhiza herb.
研究领域:
中药学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Heba Emam,Rashid Al Hajri,Nazir Ahmad,Fatma M. Elantabli,M. El-Rabiei,Abdelwahab Hassan,Mohammed Al Abri,Hussein A. Younus
The quest for an efficient and sustainable electrocatalyst for hydrogen evolution reaction (HER) using earth-abundant elements is crucial for cost-effective and environmentally friendly hydrogen production. While many catalysts show good activity and stability in strongly basic conditions, fewer materials are effective under neutral conditions, which are more practical for electrolyzer operations. This study introduces a dinuclear copper catalyst, [Cu 2 (μ-OH) (μ-NO 3 ) (L) 2 ], where L is the Schiff base ligand derived from salicylaldehyde and histidine amino acid (Complex 1 ), for HER in both aqueous and non-aqueous environments. In non-aqueous conditions, with acetic acid as a proton source, the catalyst exhibits outstanding HER performance, achieving an overpotential of 170 mV. At an acid concentration of 0.086 M, it achieves a catalytic current of ∼17.5 mA cm −2 at an overpotential of 0.52 V. Remarkably, in fully aqueous neutral conditions, Complex 1 reaches a significant current density with an i c /i p ratio of ∼82 at a scan rate of 1.0 V s −1 , and an apparent rate constant ( k obs ) for electrocatalytic HER of ∼13,200 s −1 . The catalyst also shows excellent activity in 0.1 M H 3 PO 4 , with low overpotentials of ∼150 mV at 2.0 mA cm⁻ 2 and 270 mV at 10.0 mA cm⁻ 2 . In controlled potential electrolysis (CPE), the catalyst maintains stable catalytic currents of 25 mA cm⁻ 2 and 75 mA cm⁻ 2 for 18–28 h at a potential of 0.590 V vs. RHE in neutral and acidic conditions, respectively, without noticeable decrease in catalytic current. Detailed characterizations confirm the molecular integrity of the catalyst and its predominantly homogeneous catalytic mechanism.
研究领域:
化学
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材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·Vol. 14
·期 9
·2302532
·
IF 24.4
Pan Luo,Honglei Wang,Xue Wen,Xianzhu Luo,Peng Xu
The electrocatalytic preparation of hydrogen at different pH values not only achieves excellent device performance but also promotes the application of reactive oxygen species (ROS) clearance and hydrogen anti-inflammation. However, it is difficult to develop materials that simultaneously achieve these excellent properties. Herein, the preparation of beaded necklace-like Co 9 Se 8 microspheres using a general and facile synthetic strategy is reported. The Co 9 Se 8 -modified electrode has three applications: efficient water splitting for enhanced performance, ROS scavenging, and hydrogen anti-inflammatory activity. Experiments, high-angle-annular-dark-field scanning transmission electron microscopy, and density functional theory calculations indicate that the reconstructed Co(OH) 2 plays a vital role in the oxygen evolution reaction and that the transition from *O to *OOH is the actual rate-determining step. The Co 9 Se 8 material, with its unique beaded necklace-like structure, exhibits exceptional hydrogen production capabilities in phosphate buffer solution (pH 7.4). In particular, hydrogen produce under neutral conditions can effectively reduce ROS levels and significantly inhibit inflammation-related pathological processes, playing a unique antioxidant and anti-inflammatory role at the cellular level. The obtained results indicate that the as-synthesized Co 9 Se 8 is more suitable for water splitting, ROS scavenging, and hydrogen anti-inflammatory applications, outperforming other transition metal electrodes and rendering practical industrial and clinical applications.
研究领域:
材料科学
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生物医学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
SOLVENT EXTRACTION AND ION EXCHANGE
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2022
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IF 3.695
Huifang Xing,Liangrong Yang,Lu Wang,Mengfang Li,Jiemiao Yu,Diannan Lu,Gang Ye,Huizhou Liu
The effect of ion species and concentration on the extraction percent of Cs+ by 1,3-Diisopropoxycalix [4] arenecrown-6 (BPC6) in octanol/water solvent extraction system has been studied by molecular dynamics simulations and experiments. The results show that the anionic species play an important role on the enhancement of the extraction percent of Cs+. Specifically, the order in which anions promote the extraction percent is different at different total anion concentrations. At a relatively low anion concentration of 0.5 M, the extraction percent follows the sequence: ClO4−> I−> NO3−> Br−> Cl−> SO42−> F−. At a relatively high concentration of 2 M, the extraction percent of Cs+ follows the following sequence: I−> ClO4−> Br−~ NO3−> Cl−> SO42−> F−. It is indicated that the extraction percent is dominated by the anion’s interface propensity, which is the probability of anion distribution in the interface compared to the water phase. However, at low concentration of anions, strong coordination effect of NO3− promotes the extraction effect compared to Br−. At the high anion’s concentration, the stronger salting-out capacity of Br− leads to a considerable increase of extraction percent. In addition, the cations also slightly affect the extraction percent. The extraction percent is affected by both cations’ concentration and the salt-out effect. On this basis, a neutral Cs+ extraction system has been established, and one stage extraction percent could reach 62.5%.
研究领域:
化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2019
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IF 7.913
Wei Xiang,Tao Zhou,Yifan Wang,Mingjie Huang,Xiaohui Wu,Juan Mao,Xiejuan Lu,Beiping Zhang
This study has demonstrated that hydroxylamine (HA) could greatly enhance Cu nanoparticles (nCu) in activating molecular oxygen and significantly elevate the diclofenac (DCF) degradation rate about two orders of magnitude in neutral circumstances. Effects of several important parameters on the DCF degradation such as nCu loading, HA dosage, pH and reaction temperature were investigated in the nCu/HA/O 2 system. Multiple examinations revealed that the reactive Cu(III) species instead of OH• would be predominant in the nCu/HA/O 2 system, despite their similar DCF degradation pathways. Based on a HA-enhanced copper cycle depending on the pristine Cu 0 @Cu(I) (hydro)oxides core-shell structure, the heterogeneous-homogeneous reaction mechanism was proposed. It included solid-liquid interfacial and bulk reactions, e.g. heterogeneous activation of O 2 by Cu(I) to produce H 2 O 2 and homogeneous Cu(I)-catalytic generation of Cu(III) from H 2 O 2 . Further quantitative investigation of the main reactive species in the cycle revealed that the Cu(I) regeneration instead of the O 2 activation would be rate-limited. Besides, nCu could be recycled to effectively degrade DCF in four consecutive cycles in the raw neural nCu/HA/O 2 system. It suggested that the nCu/HA/O 2 system with a more efficient copper cycle would be a good alternative Fenton-like system in treating neutral recalcitrant organic wastewaters.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
GEOCHIMICA ET COSMOCHIMICA ACTA
·
2017
·
IF 4.609
Peng Zhang,Songhu Yuan
Besides acidic environments, pyrite oxidation also occurs in circumneutral environments, such as well-buffered marine and estuarine sediments and salt marshes where low-molecular-weight organic acids (LMWOAs) (e.g., citrate and oxalate) prevail. However, the production of hydroxyl radicals ( OH) from pyrite oxidation by oxygen (O 2 ) in these circumneutral environments is poorly understood. In this study, OH production was measured during the abiotic oxidation of pyrite by O 2 under circumneutral conditions. A pyrite suspension (50 g/L pyrite) that was buffered at pH 6–8 was exposed to air for oxygenation in the dark. Benzoate (20 mM) was added into the suspension to trap OH. At pH 7, the cumulative OH reached 7.5 μM within 420 min in the absence of LMWOAs, whereas it increased to 14.8, 12 and 11.2 μM in the presence of 1 mM ethylenediaminotetraacetate, citrate and oxalate, respectively. When the citrate concentration, which serves as a LMWOAs model, was increased from 0.5 to 5 mM, the cumulative OH increased from 10.3 to 27.3 μM within 420 min at pH 7. With the decrease in pH from 8 to 6, the cumulative OH increased from 2.1 to 23.3 μM in the absence of LMWOAs, but it increased from 8.8 to 134.9 μM in the presence of 3 mM citrate. The presence of LMWOAs enhanced the OH production from pyrite oxidation under circumneutral conditions. In the absence of LMOWAs, OH is produced mostly from the oxidation of adsorbed Fe(II) by O 2 . In the presence of citrate, OH production is attributed mainly to the oxidation of Fe(II)-citrate − by O 2 and secondarily to the oxidation of H 2 O on surface-sulfur defects. The acceleration of pyrite oxidation by Fe(III)-citrate increases OH production. Fe(II)-citrate − is generated mainly from the complexation of adsorbed Fe(II) by citrate and the reduction of Fe(III)-citrate, and the generation is suppressed by the oxidation of adsorbed Fe(II). Fe(III)-citrate is generated predominantly from Fe(II)-citrate − oxidation. Most soluble Fe 3+ that is produced from pyrite oxidation hydrolyzes to Fe(III) hydroxide. Kinetic models that were developed according to the proposed mechanisms identified the relative importance of each reaction for OH production. Using the kinetic model, the oxidation efficiencies of the redox-active substances that react with OH at different reaction-rate constants were estimated in the presence of 1 mM citrate. This study presents on the overlooked role of LMWOAs in enhancing OH production from pyrite oxidation by O 2 in pyrite-rich circumneutral environments, such as marine and estuarine sediments and salt marshes.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zhewen Shao,Kexin Xiang,Shuchang Liu,Feng Hong,Ye Gao,Enhong Lei,Jinping Jia,Yingping Huang
Presently, fast degradation of organic wastewater has been achieved by the synergetic method of hydrodynamic cavitation and H2O2 at a laboratory scale, while the physico-chemical effect, especially the turbulence characteristics on the degradation process remains lacking. This paper presents investigation on the degradation of dyeing wastewater containing methylene blue (MB) under neutral condition, within a vortex-based hydrodynamic cavitation (VBHC) reactor. Operating conditions are firstly optimized and then used to collaborate with H2O2 to study the synergetic effects of this hybrid treatment method. The turbulence characteristics are subsequently obtained by a computational fluid dynamics (CFD) simulation, and the correlation between them and the degradation process of MB is revealed. The results indicate that the highest degradation rate of 91.95 % is achieved under optimal conditions. Higher inlet pressure (4.5 bar) owns the thickest vapor volume fraction, greatest vapor transfer rate, and largest size of cloud cavity in the vortex core region, indicating the strongest cavitation intensity; meanwhile, moderate solution temperature (30 ℃) also favors for the greatest cavitation intensity inside the reactor. The optimal cavitation intensity activates the considerable production of reactive oxygen species, and results in good consistency with the MB degradation performance, which predominately occurs in the annular region around the vortex rope. This research unveils the rationale behind the physical essences of the VBHC process and its influence on the degradation efficacy of MB, which can provide reliable guidance for further development of cavitational reactors to degrade organic pollutants by the VBHC/H2O2 hybrid treatment method.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhi-Hui Huang,Jia-Ming Liu,Zhi-Yong Ji,Peng Yuan,Xiao-Fu Guo,Shu-Ming Li,Hong Li,Jun-Sheng Yuan
Electro-Fenton (EF) generally relies on the addition of iron in acidic conditions, which caused an increase in cost and secondary pollution. In this paper, Fe 3 O 4 was in-situ loaded on the surface of the graphite felt (GF) electrode by a moderate solvothermal synthesis method. The modified electrode (Fe 3 O 4 /GF) could be used in a wide pH range (acid, and even neutral conditions), and Fe dissolution was not detected under neutral conditions. Compared with the pre-activated graphite felt electrode (aGF), the Fe 3 O 4 /GF electrode could directly utilize the generated hydrogen peroxide (H 2 O 2 ) to obtain more hydroxyl radicals (•OH). The influence of electrolyte types was also investigated, and the results showed unstable or reductive electrolytes were not conducive to the degradation of levofloxacin (LEV). The Fe 3 O 4 /GF electrode had good reusability, and could maintain a LEV degradation ratio of over 70% during 6 cycles. The degradation effect of EF with unmodified GF is poor under neutral conditions, but the degradation with the Fe 3 O 4 /GF cathode is continuous and has a high total organic carbon (TOC) removal ratio of 81.4% at 6 h. The Fe 3 O 4 /GF cathode is conducive to promote the application of EF technology in the field of wastewater treatment, especially under neutral conditions.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2022
·
IF 25.832
Tao Liu,Yuxin Chen,Yaming Hao,Jianxiang Wu,Ran Wang,Limin Gu,Xuejing Yang,Qiang Yang,Cheng Lian,Honglai Liu,Ming Gong
The ion-enriched electrode-electrolyte interface is a unique characteristic of electrocatalytic reactions that can effectively tune the local chemical environment. In this study, we discovered a strong synergy between borate and fluoride anions for water oxidation in neutral conditions. Under an optimal ratio of the two anions, the water oxidation current significantly outperforms the individual counterparts by almost an order of magnitude. This synergy was greatly attributed to the hierarchical anions at the interface, with borate approaching the surface and fluoride extending out, as revealed by in situ surface-enhanced Raman spectroscopy and molecular dynamics simulation. This hierarchical anion arrangement created two kinetics regions, with one borate-dominating region to lower the onset potential and one fluoride-dominating region to sustain a larger current. Using the synergized electrolyte, a low-cost and facilely synthesized Co(OH) 2 electrode could achieve an outstanding performance of 100 mA/cm 2 at 1.791 V versus RHE under pH = 7.87 with a 2-week-long durability.
研究领域:
电化学
·
材料科学
·
催化反应
✓ 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）