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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

In situ-generated H2O2 with NCQDs/MIL-101(Fe) by activating O2: A dual effect of photocatalysis and photo-Fenton for efficient removal of tetracyline at natural pH

Yuanhong Xie,Chenrui Liu,Dejian Li,Yun Liu

Herein, a novel composite of MIL-101(Fe) loaded with nitrogen doped carbon quantum dots (NCQDs/MIL-101(Fe), denoted as NQML), which can construct dual effect of photocatalysis and photo-Fenton for organic pollutants removal, was prepared by solvent impregnation method. Characterization methods proved that NQML had been synthesized successfully. Additionally, the adding volume of NCQDs could effectively influence the photocatalytic activities of NQML-x composites (x represents the adding volume of NCQDs) for tetracycline (TC) degradation, and NQML-8 exhibited the optimum photocatalytic performance among the studied catalysts upon visible light illumination under natural pH, which can completely degrade TC within 180 min. By comparison, the TC degradation kinetic constant in the system with NQML-8 was as 15.85 and 8.24 folds of that in the NCQDs and MIL-101(Fe) systems, respectively. The mechanism study proved that the enhanced photocatalytic performance of NQML was resulted from the visible light up-conversion property, electron-hole separation and transfer capacity of NCQDs. Meanwhile, NQML could not only produce h + but also lead to in-situ generation of O 2 - and H 2 O 2 by activation of O 2 under visible light. The generated H 2 O 2 could react with Fe(II) in MIL-101(Fe) to produce OH so as to construct a dual effect of photocatalysis and photo-Fenton in TC removal.

研究领域: 环境科学 · 材料科学 · 化学工程 · 光化学
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ACS Nano · 2024 · IF 15.8

Microenvironment-Modulating Adsorption Enables Highly Efficient Lithium Extraction under Natural pH Conditions

Yu Han,Jiaxiang Ma,Dongqing Liu,Yan Yang,Tao Zhang,Min Wang,Daxin Liang,Liping Wen,Jun Ma,Wei Wang

Ion-sieve adsorbents are effective materials in practical applications for extracting liquid lithium. However, it is greatly suppressed in adsorption capacity and selectivity (Li/Mg) under natural near-neutral conditions of seawater or salt lakes, due to the interference of in situ released H+ and Mg2+ impurity. This paper proposes an adsorbent with a microenvironment-modulating function as a solution. The introduction of quaternary ammonium groups into the carrier accelerates the migration of H+, while preventing the diffusion of Mg2+ by electrostatic repulsion. Besides, it can also prestore OH–, effectively consuming the generated hydrogen ions in situ. Based on the rational design, the alkali consumption of the microenvironment-modulating strategy is dramatically reduced to 1/144 of the traditional alkali-adding method. Additionally, adsorption performance is significantly promoted under natural pH conditions, with a maximum 33 times higher separation factor (selectivity) and 4 times higher adsorption capacity than commercial ion-sieve adsorbents. This development indicates the feasibility of using microenvironment modulation for effective lithium extraction and inspires the development of next-generation high-performance adsorbents.

CAS / MDL: 554-13-2 598-62-9
研究领域: 材料科学 · 环境工程 · 化学工程 · 可持续能源
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2019 · IF 7.149

Cathode-Introduced Atomic H* for Fe(II)-Complex Regeneration to Effective Electro-Fenton Process at a Natural pH

Xiao-Cheng Liu,Wen-Qiang Li,Yi-Ran Wang,Guan-Nan Zhou,Yi-Xuan Wang,Chuan-Shu He,Gong-Ming Wang,Yang Mu

Promotion of iron solubility using ligands is the preliminary step in the homogeneous electro-Fenton (EF) process at a mild pH, but the chelate efficiencies of most organic ligands are unsatisfactory, resulting in insufficient Fe(II) availability. In this study, atomic H* was, for the first time, introduced to the EF process to accelerate the regeneration of the Fe(II)-complex at a mild pH using a Ni-deposited carbon felt (Ni-CF) cathode. The introduction of atomic H* significantly elevated total organic carbon (TOC) abatement of ciprofloxacin (CIP) from 42% (CF) to 81% (Ni-CF) at a natural pH. In the presence of humic acids (HAs), atomic H* introduced via Ni-CF enhanced the CIP degradation rate to 10 times that of the CF at a mild pH. The electron spin resonance (ESR), density functional theory (DFT) calculations, electrochemical characterization, and in situ electrochemical Raman study clearly demonstrated that the atomic H* generated from the Ni-CF cathode was highly efficient at reducing Fe(III)-complexes at a natural pH. Additionally, the Ni-CF could generate atomic H* without significant nickel leaching. Thus, the atomic H* could continuously facilitate iron cycling and, consequently, enhance pollutant mineralization via the homogeneous EF process at a mild pH in an environmentally friendly manner.

CAS / MDL: 101385-69-7 7647-01-0
研究领域: 环境科学 · 化学工程 · 水处理 · 电化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Degradation of Cephalosporin C using MOF-derived Fe-Co bimetal in carbon cages as electro-Fenton catalyst at natural pH

Yaoyu Zhou,Jianlong Wang

Developing high performance electrocatalysts for effective antibiotics elimination for heterogeneous electro-Fenton (Hetero-EF) process is still a challenge. This work synthesized iron/cobalt bimetallic N doped graphitic carbon cages (Fe x Co@NC) from ZIF-8@ZIF-67-Fe dual MOF composite for Cephalosporin C (CEP-C) degradation in the Hetero-EF system at a wide pH range. Results indicated that CEP-C degradation rate and total organic carbon (TOC) removal efficiency by Fe 40 Co@NC catalyst were as high as 82.45% (60 min) and 61.35% (240 min) at natural pH, respectively. The unique structure with FeCo bimetal encapsulated inside the N doped graphitic carbon cages enabled Fe 40 Co@NC to show excellent catalytic reactivity for H 2 O 2 activation. The generated M (•OH) and •OH all contributed to CEP-C degradation. The synergistic effects of Co 0 /Co 2+ /Co 3+ and Fe 0 /Fe 2+ /Fe 3+ cycles made Fe 40 Co@NC catalyst to continuously activate H 2 O 2 . Moreover, Fe 40 Co@NC catalyst showed good stability in consecutive cycles, and could still remain excellent reactivity when applied for CEP-C degradation from the real CEP-C fermentation residue supernatant. Furthermore, a possible CEP-C degradation pathway was proposed based on the identified intermediates.

CAS / MDL: 75-05-8 64-18-6
研究领域: 环境科学 · 化学工程 · 材料科学 · 催化
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