CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Hang Xu,Mingjing Ge,Yin Liu,Chen Yao,Houzhen Zhou,Mingmei Ding,Yang Li
Singlet oxygen ( 1 O 2 ) is an electrophilic oxidant capable of selectively eliminating contaminants in complex wastewater, which is highly expected in environmental remediation. However, due to the limitations in synthesizing catalysts with well-defined adsorption and active sites, the efficient and selective generation of 1 O 2 remains challenging. Herein, isolated Ru-O 3 moiety decorated two-dimensional Ti 3 C 2 T x catalysts (Ru-SA/Ti 3 C 2 T x ) were prepared to regulate 1 O 2 generation via peroxymonosulfate (PMS) activation. The constructed catalysts with asymmetric dual-metal structures (Ti-O-Ru) exhibited surprising mass activity of 1.4 × 10 4 min −1 ·mol −1 with a high 1 O 2 generation selectivity of 98.3 %. Mechanism inquiry indicated that the enhanced adsorption and electron transfer between PMS and Ru-SA/Ti 3 C 2 T x attributed to the synergistic effect of the strong adsorption at the Ru sites and the rapid electron transfer in the asymmetric Ti-O-Ru structures. Theoretical calculations demonstrated that Ru-O 3 moiety decreased the formation energy barrier of key intermediate *O, thus converting to a 1 O 2 -dominated oxidation path. Two possible degradation pathways of tetracycline hydrochloride (TCH) were proposed by gas chromatography-mass spectrometry (GC–MS), and the toxicities of intermediates were significantly decreased due to the strong electrophilic attack of 1 O 2 . This study deepened the understanding of the specific contribution of individual sites in multi-site synergistic, which furnished implications for the design and optimization of Fenton-like catalysts.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yun Liu,Guijiang Liu,Yanyan Yu,Yunying Wang
The burgeoning interest in single atom catalysts (SACs) stems from their exceptional oxidase-mimicking capabilities, driving substantial advancements in this field. Nevertheless, a critical knowledge gap remains regarding the influence of Zn incorporation on the oxidase-like activity of atomically dispersed Fe-N-C catalysts. This study successfully synthesized and comprehensively characterized three distinct SACs (FeZn SAC-N@C, Fe SAC-N@C, and Zn SAC-N@C) using TEM, HAADF-STEM, XRD, XPS, BET, ICP-MS, and XAFS techniques. Activity assays revealed that FeZn SAC-N@C exhibited the highest oxidase-mimicking activity, with Fe SAC-N@C displaying moderate activity, whereas Zn SAC-N@C did not exhibit oxidase-like behavior. The superior oxidase-like activity of FeZn SAC-N@C is attributed to its enhanced O 2 activation capacity, characterized by a high free energy of 0.90 eV in the rate-determining reaction step, surpassing those of Fe SAC-N@C (0.85 eV) and Zn SAC-N@C (0.71 eV). EPR and DFT calculations elucidated the catalytic mechanism of FeZn SAC-N@C, involving the generation of O 2 − radicals. As a proof-of-concept, FeZn SAC-N@C demonstrates potential as a colorimetric sensor for detecting ascorbic acid and nitrite, achieving a limit of detection of 0.77 μM for ascorbic acid and 0.16 μM for nitrite. These findings open a new avenue for configuring bimetallic atomically dispersed catalysts with oxidase-like activity in future research.
研究领域:
生物化学
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材料科学
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催化反应
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DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Wendi Guo,Zehui Sun,Meng-Jiao Xu,Kaizhi Wang,Mugeng Chen,Conglin Zhu,Heyong He,Yong-Mei Liu,Yong Cao
The efficient and environmentally friendly removal of halogen substituents from organic substances is crucial for reducing the ecological and health hazards posed by persistent halogenated compounds. In this regard, we introduce CoN3P1@NP-PC, a novel asymmetric CoN3P1 single-atom catalyst, which demonstrates outstanding efficiency in transfer hydrodehalogenation (HDH) using just two equivalents of HCOONH4 as a benign and effective reducing agent. This catalyst was synthesized through a simple post-implantation method, capitalizing the high porosity and large surface area of ZIF-8 precursors. Extensive characterization via a range of spectroscopic and microscopic techniques confirmed CoN3P1@NP-PC's superior atomic dispersion and asymmetric structural integrity, which was more favourable for HCOONH4 activation allowing facile generation of hydrogen radical along with electron transfer. In our comprehensive evaluation, CoN3P1@ NP-PC displayed outstanding versatility for transformation of a diverse array of halogenated substrates, efficiently processing compounds with varied functional groups and complex molecular structures. Notably, CoN3P1@NP-PC proved particularly effective in breaking down brominated flame retardants such as 2,4,6-tribromophenol and tetrabromobisphenol A, reinforcing its potential as a powerful tool for ecological restoration and pollution control.
研究领域:
催化化学
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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
Sustainability
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2025
·Vol. 17
·期 6
·2469
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IF 3.3
Huidong Tang,Jiacheng Bao,Chen Liu,Yuwen Deng,Yixing Ma,Lei Shi,Shuangyou Bao,Kai Li,Ping Ning,Xin Sun
In pursuing sustainable environmental solutions, the concept of ‘waste to treasure’ has emerged as a promising approach. In this study, a new process is proposed to combine solid copper slag with hydrogen peroxide (H2O2) to remove nitrogen oxides (NOx) from acidic exhaust gases, thus effectively utilizing waste materials. Firstly, different smelting slags were screened to determine the catalytic potential of copper slag for hydrogen peroxide. Subsequently, the catalytic activity of the copper slags at various stages of the copper smelting process was thoroughly evaluated and optimized. In addition, a multifactorial evaluation of slow-cooled copper slag catalysts for removing NOx was carried out. Preliminary indications are that the iron phase in the copper slag is identified as the main source of catalytic activity sites. The results suggest that Fe2+/Fe3+sites on the surface of the Fe phase in the slow-cooled copper slag may be crucial in improving the NOx removal efficiency. The main reactive oxygen species detected in the system were ·OH, ·O2⁻, and1O2. In addition, the transformation products, formation pathways, and reaction mechanisms of NO in the liquid phase were initially investigated and determined. This study provides a green and sustainable path for the utilization of solid waste and management of atmospheric fumes in the non-ferrous metal industry and offers new perspectives to address environmental challenges in industrial processes.
研究领域:
环境科学
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冶金工程
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zixin Zhang,Guohe Huang,Yongping Li,Yao Yao,Peng Zhang,Xiujuan Chen,Shaojie Ren,Yifei Luo,Yuanzheng Zhang
Rendering heterogeneous electro-Fenton (hetero-e-Fenton) reactivity is a promising strategy to address the bottlenecks of low-pressure membranes (LPMs), such as the poor ability to remove small-molecular organic pollutants and membrane fouling. However, hetero-e-Fenton catalysis usually suffers from the limitation of the sluggish redox cycle of Fe(III)/Fe(II). Herein, we reported an electrocatalytic ceramic microfiltration membrane functionalized with CuFe 2 O 4 nanoparticles supported by nitrogen-doped carbon nanotubes (NCNTs). The Fe(II) and Cu(I) sites on the CuFe 2 O 4 decomposed the H 2 O 2 generated by NCNTs into ·OH. The electron transfer from the conductive NCNTs support and reducing agent Cu(I) to Fe(III) enabled an effective Fe(II) regeneration. Moreover, the N species in NCNTs enhanced the interfacial interaction between CuFe 2 O 4 nanoparticles and the NCNTs support, expediting the Fe(III)/Fe(II) redox cycle by promoting the interfacial electron transfer. At near-neutral pH, the electrocatalytic membrane delivered excellent tetracycline removal kinetics (0.0134 min −1 ) and significantly alleviated the organic fouling on the membrane surface and in the pores. The membrane also exhibited good stability, reusability, and permeate water safety. These findings shed new light on the development of next-generation water treatment membranes with catalytic oxidation capabilities.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
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
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Zhenkai Wang,Yifan Li,Yanfang Su,Sheng-Peng Sun,Xiaoning Wang,Zhangxiong Wu,Winston Duo Wu,Xiao Dong Chen
Catalytic membrane integrating membrane filtration and advanced oxidation in one single-step is promising in addressing emerging micropollutants issue in water, the challenges in catalytic activity and stability still limit their practical application. This study successfully anchored highly stable Fe–Mn bimetallic catalyst (FMBC) in Al 2 O 3 -based microfiltration and ultrafiltration ceramic membranes channel (named as FMBC@Al 2 O 3 -MF or UF) via a novel in situ fabrication strategy. Characterization results revealed that FMBC was anchored on the membrane channel wall of Al 2 O 3 -MF/UF, which enabled boosting Oxone activation to generate sulfate radical and hydroxyl radical at circumneutral pH (e.g., 7.0–9.0) and with great stability. Notably, FMBC@Al 2 O 3 -UF exhibited a remarkable activity and anti-interference capability in actual water matrices, which resulted in efficient degradation of emerging micropollutants such as carbamazepine, crotamiton, diethyltoluamide, gemfibrozil and ibuprofen in lake water and municipal wastewater treatment plant secondary effluent at environmentally relevant concentrations. Moreover, FMBC@Al 2 O 3 -MF/UF also displayed high cleaning efficiency toward natural organic matter (NOM) and effluent organic matter (EfOM) fouling via Oxone activation. Besides, the intermediates of carbamazepine degradation were identified, and most of them had decreased aquatic toxicity based on Ecological Structure Activity Relationship (ECOSAR) prediction. The high activity, stability and environmentally friendly property of the as-prepared FMBC@Al 2 O 3 -MF/UF make them promising application for advanced treatment of emerging micropollutants in water.
研究领域:
环境科学
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水处理技术
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yan Ke,Mingzhu Yuan,Xinglong Li,Yuan Liu,Yangyang Li,Yuanxu Liu,Xiangang Lin,Qinghua Liu,Yupeng Yuan
Improving electron delocalization and optical absorption properties of graphitic carbon nitride (g-C 3 N 4 ) is essential for enhancing the performance of photocatalytic wastewater treatment. Herein, an enhanced electron delocalization with activation n-π∗ electronic transitions of g-C 3 N 4 (TCN m ) by embedding electron-rich pyrimidine units into the g-C 3 N 4 skeleton was successfully fabricated. Experimental characterizations and density functional theory calculations demonstrated that the precise incorporation of pyrimidine units into the g-C 3 N 4 skeleton reduces the degree of overlap of positive and negative charge centers, enhances the delocalization of conjugate electrons, and facilitates carrier separation. Furthermore, this novel structure introduced additional n-π∗ electronic transitions, extending the light-absorbing edge beyond 700 nm. As a result, after 60 min of light irradiation, TCN m exhibited the highest kinetic constant (0.0287 min −1 ) in the degradation of tetracycline, which was ∼3.8 times higher than that of pristine g-C 3 N 4 . In particular, the optimal antibacterial rate for Staphylococcus aureus reached 88.3% after 4 h of light exposure. These findings illustrate the remarkable potential of TCN m in addressing antibiotic and microbial contamination in water.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Sustainability
·
2024
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IF 25.7
Zhang Gong,Li Binggong,Shi Yanfeng,Zhou Qi,Fu Wen-Jie,Zhou Gang,Ma Jun,Yin Shuo,Yuan Weihao,Miao Shiyu,Ji Qinghua,Qu Jiuhui,Liu Huijuan
Electrocatalytic nitrate reduction has great potential for simultaneously achieving ammonia recovery and nitrate-rich wastewater treatment. However, the complexity of wastewater matrices has long hampered its implementation and commercialization in the wastewater treatment industry. Here we develop a membrane-free electrochemical system, called electrochemical NO 3 − conversion synchronized with NH 3 recovery (ECSN), which synchronizes nitrate reduction with ammonia recovery for treating real nitrate-rich wastewater. Key components of this system include a 3D-printed metallic glass decorated Cu–Ni (MPCN) working electrode bearing good corrosion resistance and a UV-assisted stripping unit. When treating real electroplating wastewater, the ECSN system converts over 70% of nitrate into high-purity ammonia chloride. Long-term stability test demonstrates the robustness of the ECSN system in treating real wastewater. Further, the economic feasibility and environmental benefits of this system are evidenced by technoeconomic analysis and life-cycle analysis. Overall, this work brings the electrocatalytic nitrate reduction process one step closer to practical application, contributing to both environmental protection and the circularity of anthropogenic nitrogen flow.
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
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Yi,Wang Shuo,Fu Yunfan,Sang Jiaqi,Wei Pengfei,Li Rongtan,Gao Dunfeng,Wang Guoxiong,Bao Xinhe
Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory electrocatalytic activity and long-term stability. Herein we achieve high-rate ammonia electrosynthesis using a stable amorphous/crystalline dual-phase Cu catalyst. The ammonia partial current density and formation rate reach 3.33 ± 0.005 A cm −2 and 15.5 ± 0.02 mmol h −1 cm −2 at a low cell voltage of 2.6 ± 0.01 V, respectively. Remarkably, the dual-phase Cu catalyst can maintain stable ammonia production with a Faradaic efficiency of around 90% at a high current density of 1.5 A cm −2 for up to 300 h. A scale-up demonstration with an electrode size of 100 cm 2 achieves an ammonia formation rate as high as 11.9 ± 0.5 g h −1 at a total current of 160 A. The impressive electrocatalytic performance is ascribed to the presence of stable amorphous Cu domains which promote the adsorption and hydrogenation of nitrogen-containing intermediates, thus improving reaction kinetics for ammonia formation. This work underscores the importance of stabilizing metastable amorphous structures for improving electrocatalytic reactivity and long-term stability.
研究领域:
材料科学
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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
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Li Tu,Shengqiang Chen,Zhikang Yuan,Yeqi Xiong,Bingkun Luo,Ying Chen,Zhenqing Hou,Sunkui Ke,Naibo Lin,Chao Li,Shefang Ye
Nanozymes, as nanomaterials with natural enzyme activities, have been widely applied to deliver various therapeutic agents to synergistically combat the progression of malignant tumors. However, currently common inorganic nanozyme-based drug delivery systems still face challenges such as suboptimal biosafety, inadequate stability, and inferior tumor selectivity. Herein, a super-stable amino acid-based metallo-supramolecular nanoassembly (FPIC NPs) with peroxidase (POD)- and glutathione oxidase (GSHOx)-like activities was fabricated via Pt 4+ -driven coordination co-assembly of l -cysteine derivatives, the chemotherapeutic drug curcumin (Cur), and the photosensitizer indocyanine green (ICG). The superior POD- and GSHOx-like activities could not only catalyze the decomposition of endogenous hydrogen peroxide into massive hydroxyl radicals, but also deplete the overproduced glutathione (GSH) in cancer cells to weaken intracellular antioxidant defenses. Meanwhile, FPIC NPs would undergo degradation in response to GSH to specifically release Cur, causing efficient mitochondrial damage. In addition, FPIC NPs intrinsically enable fluorescence/photoacoustic imaging to visualize tumor accumulation of encapsulated ICG in real time, thereby determining an appropriate treatment time point for tumoricidal photothermal (PTT)/photodynamic therapy (PDT). In vitro and in vivo findings demonstrated the quadruple orchestration of catalytic therapy, chemotherapeutics, PTT, and PDT offers conspicuous antineoplastic effects with minimal side reactions. This work may provide novel ideas for designing supramolecular nanoassemblies with multiple enzymatic activities and therapeutic functions, allowing for wider applications of nanozymes and nanoassemblies in biomedicine.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）