WATER ENVIRONMENT RESEARCH
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2025
·Vol. 97
·期 5
·e70070
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IF 1.9
Fanye Wang,Jinnan Liu,Jingrui Liu,Xinchao Ruan,Xiaojun Yang
The widespread use of tetracycline has made the efficient and environmentally friendly treatment of tetracycline-contaminated wastewater a pressing issue in environmental management. This study synthesized high-purity and uniformly mixed Cu 0 /CuFeO 2 composite materials using a one-step hydrothermal method, aiming to enhance the catalytic activation of peroxymonosulfate (PMS) through the synergistic effect of zero-valent metal and bimetallic compounds. The Cu 0 /CuFeO 2 composite demonstrated exceptional PMS activation performance, achieving 84% tetracycline hydrochloride (TCH) degradation within 1 min and 91% degradation within 20 min. The degradation process involved the synergistic action of •OH, SO 4 •− , 1 O 2 , and electron transfer. The degradation intermediates of TCH were identified using high-performance liquid chromatography–mass spectrometry (HPLC-MS), and four potential degradation pathways were proposed. Furthermore, Cu 0 /CuFeO 2 exhibited robust degradation performance across a wide pH range and maintained high efficiency in complex aqueous environments. Even after five cycles, the composite retained 78% of its degradation efficiency, demonstrating excellent stability and reproducibility in the degradation of TCH using the Cu 0 /CuFeO 2 /PMS system. Practitioner Points A high-purity and uniformly mixed Cu 0 /CuFeO 2 composite was synthesized. Robust catalytic activity and stability was observed for the synthesized catalyst. Synergistic contributions from •OH, SO 4 •− , 1 O 2 , and e − resulted in TCH degradation. Four potential TCH degradation pathways were derived. Graphical A Cu 0 /CuFeO₂ composite was synthesized, characterized, and optimized to activate peroxymonosulfate (PMS) for degrading tetracycline hydrochloride (TCH) and related antibiotics. In this system, Cu 0 acted as an electron donor, facilitating electron transfer through the redox cycling of metal ions. This process sustained the continuous generation of reactive oxygen species—including •OH, SO₄•⁻, and ¹O₂—as well as electrons, thereby promoting the efficient degradation of TCH. Furthermore, four potential degradation pathways were proposed based on the identified degradation intermediates.
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
PubMed
高影响因子
CATALYSIS TODAY
·
2024
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IF 5.2
Ziheng Zhen,Antai Li,Youwei Yang,Ying Hu,Jing Lv,Shouying Huang,Yue Wang,Xinbin Ma
Cu/CeO 2 catalysts have been wildly used for the hydrogenation of carbon-oxygen bonds reactions due to their excellent catalytic performance. It is widely accepted that the Cu 0 -Cu σ+ interface could be the primary active sites during the reaction, but how to form and maintain highly dispersed such species remains challenging under the reaction conditions of high temperature and H 2 partial pressure. In this work, we proposed an effective strategy to construct stable Cu 0 -Cu σ+ interface sites over the Cu/CeO 2 catalysts by in situ N 2 O-involved oxidation treatment . It was evidenced that the sequential oxidation-reduction by N 2 O and H 2 broke the grain boundaries of Cu nanoparticles and therefore facilitated the formation of the active Cu 0 -Cu σ+ sites, leading to an enhanced activity. However, a rapid deactivation was observed after this temporary enhancement due to the aggregation of copper species. We further introduced some additional cerium species during catalyst preparation. The 16Cu/CeO 2 -1Ce catalyst prepared by post-impregnation of 1 wt% cerium achieved a stable performance of 90.6% MA conversion after the N 2 O-involved oxidation treatment, which was much higher than that of 26.2% over the 16Cu/CeO 2 catalyst. It was demonstrated that the strong interaction between the formed CeO 2 and reconstructed Cu species prevented the metal sintering and increased the fraction of the Cu 0 -Cu σ+ sites. This method that combined in situ N 2 O-involved oxidation treatment and cerium modification may offer potential in engineering stable active sites for high-performance catalysts in the hydrogenation of carbon-oxygen bonds.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Xiuting Wu,Zefeng Zheng,Liang Ma,Changsong Hu,Yunhong Pi,Tiejun Wang
The aqueous-phase reforming of methanol(APRM)via non-precious metal heterogeneous catalysts is highly desirable, but challenging. Herein, we report a highly efficient copper catalyst encapsulated by chitosan-glucose (CS-G) conjugate with high metal loading of 35 wt% for H 2 generation from APRM. The optimized Cu@CS 19 -G 1 -300 catalyst exhibited exceptional activity of 1.39 × 10 5 μmol H2 /g cat /h at low temperature of 210 °C, which was ∼4.5 times higher than that of commercial CuZrAl catalysts (2.88 × 10 4 μmol H2 g cat −1 h −1 ). The chitosan-glucose conjugate acted not only as the main carbon support for Cu dispersion, but also as adsorbent to stablize as many Cu ions as possible. And meanwhile, with abundant Cu + /Cu 0 interface sites due to the reducing effect of glucose, the water gas shift reaction (WGSR) was intensified and thus displayed excellent selectivity toward CO by-product. This specific catalyst construction for H 2 production from APRM exhibits great potential of on-site H 2 supply for polymer membrane fuel cells.
研究领域:
化学工程
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催化科学
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能源材料
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Jiuyu Chen,Zhiwen Liu,Baozhong Zhu,Chensheng Gao,Yunlan Sun
Radioactive iodine (I) produced in the nuclear industry can be eliminated through solid-phase adsorption. Nevertheless, conventional adsorbents suffer from limited capacity, poor selectivity, and insufficient stability. In this study, metallic copper modified nitrogen-doped carbon composites (Cu x -NC) were prepared from a pre-synthesized template of Cu 2+ -zeolite imidazole framework-8 (Cu 2+ -ZIF-8) by ball milling combined with pyrolysis processes. The surface physical and chemical properties of Cu x -NC composites were characterized, and then applied to remove iodide (I - ) in aqueous solutions. The experimental results indicated that Cu 0 introduced to nitrogen-doped carbon not only significantly enhanced I - removal but also achieved an exceptional adsorption capacity of 269.2 mg/g by incorporating 35 % copper and setting the pyrolysis temperature at 1000 °C. Notably, under acidic (pH = 3) and blown air conditions, the adsorption capacity was markedly increased, attaining 383.3 and 474.3 mg/g, respectively. The Cu 35 -NC demonstrated exceptional selectivity for I - in the presence of interfering anions such as Cl - and SO 4 2- . Mechanism studies showed that as-fabricated materials eliminated I - through adsorption and oxidation. The presence of Cu 0 particles activated molecular oxygen to release Cu + and generate H 2 O 2 , resulting in I - being adsorbed and oxidized. These findings underscore the significant potential of the economical Cu x -NC for the effective elimination of radioactive iodide.
研究领域:
环境科学
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材料科学
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核工程
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化学工程
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Qian Wang,Zhi Yu,Junting Feng,Paolo Fornasiero,Yufei He,Dianqing Li
The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C═O hydrogenation and C–O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al2O3 catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu0/Cu+ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu+/Cu0 ratio was observed; notably, Cu/ZnO-Al2O3 with higher Cu+/Cu0 ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/Al2O3 (59.6%) and Cu/MgO-Al2O3 (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu0/Cu+ site suggests that Cu0 tends to adsorb the C═O bond as well as hydrogen molecule, while the Cu+ site is preferable to adsorb and activate the C–O bond. With the synergy of dual active sites, the Cu/ZnO-Al2O3 catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.
研究领域:
催化
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化学工程
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生物化学
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材料科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2025
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IF 8
Liang Jiang,Xiaojiang Chen,Jun Liao,Lielin Wang,Yuxin Zhang,Sha Yang,Qiuyi Wang,Yaoyao Tang,Congcong Ding
Rapid and efficient removal of radioactive iodine from nuclear accidents and effluent waste was significantly essential to protect the living environment and maintain human health. The nano-zero-valent copper modified activated carbon fiber (Cu 0 @ACF) composite was successfully synthesized via an in situ self-reduction method. The structural and chemical compositions of both pristine and iodine-adsorbed samples (ACF and Cu 0 @ACF) were systematically analyzed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The coexistence of carbon and copper was verified using energy dispersive spectroscopy (EDS). The effects of modifier concentration, contact time, pH value and interfering ions on the removal of I 2 and I − were comprehensively investigated through batch experiments. The adsorption capacity of 4 wt% Cu 0 @ACF for I 2 reached 980 mg/g (C 0 = 1000 mg/L, pH = 2), and for I − was 358 mg/g (C 0 = 400 mg/L, pH = 2), significantly outperforming other reported iodine adsorbents. The kinetic studies revealed that the adsorption processes followed pseudo-second-order kinetics, while isotherm data were best described by the Langmuir model (R 2 > 0.99), indicating monolayer chemisorption. The adsorption mechanism was dominated by chemical reactions where in iodide ions (I − ) interact with the metallic nano‑copper (Cu 0 ) anchored on the ACF surface, resulting in the formation of CuI characterized by polar covalent bonding. In a word, Cu 0 @ACF showed an outstanding potential for radioactive wastewater treatment applications and this work presents a facile strategy for developing high-performance ACF-based adsorbents.
研究领域:
环境科学
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材料科学
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核工程
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化学工程
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表面化学
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产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
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2024
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IF 5.8
Jingwei Hong,Wanli Li,Jin Shang,Hiromi Yamashita,Yun Hu
Utilizing electrocatalysis to convert CO2 into high-value industrial raw materials can not only effectively reduce CO2 emissions but also achieve a closed carbon cycle. This method holds great potential for addressing global warming and alleviating the fossil fuel crisis. Here, we report a novel electrocatalyst for CO2 reduction composed of a composite material derived from Cu-MOF74 and Cu2O, synthesized under the regulation of an appropriate amount of KOH. The research results indicate that the unique Cu0/Cu+ interface in Cu-MOF74/Cu2O-350 enhances the adsorption of reaction intermediates, providing more active sites for CO2 reduction. Additionally, the moderate carbonization during the thermal treatment process increases conductivity and enriches the electrochemical active surface area, accelerating the charge transfer rate. Consequently, this composite exhibits excellent CO2 reduction performance. At -1.3 V vs. RHE, the Faraday efficiency (FE) for C2H4 production reached up to 32.48%, which was significantly higher than that of pure Cu2O-350 (9.25%) and Cu-MOF74-350 (15.52%). Even after 6 hours of reaction, the FE for C2H4 remained above 24.52%, reflecting its good stability. Furthermore, we utilized in-situ infrared spectroscopy to study the key intermediates of the relevant reduction products, inferring the possible reaction pathways for the formation of HCOOH and C2H4. This study provides a simple synthesis method for the preparation of high-selectivity MOF-derived composite catalysts for the electrocatalytic reduction of CO2 to value-added chemicals.
研究领域:
电化学
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材料科学
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环境科学
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催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yafei Qu,Wei Zheng,Peichen Wang,Hao Huang,Minxue Huang,Lin Hu,Hui Wang,Qianwang Chen
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is an effective approach to capture CO 2 and convert it into value-added chemicals and fuels, thereby reducing excess CO 2 emissions. Recent reports have shown that copper-based catalysts exhibit excellent performance in converting CO 2 into multi-carbon compounds and hydrocarbons. However, the selectivity to the coupling products is poor. Therefore, tuning CO 2 -reduction selectivity toward C 2+ products over Cu-based catalyst is one of the most important issues in CO 2 RR. Herein, we prepare a nanosheet catalyst with interfaces of Cu 0 /Cu + . The catalyst achieves Faraday efficiency (FE) of C 2+ over 50% in a wide potential window between − 1.2 V to − 1.5 V versus reversible hydrogen electrode (vs. RHE). Moreover, the catalyst exhibits maximum FE of 44.5% and 58.9% towards C 2 H 4 and C 2+ , with a partial current density of 10.5 mA cm −2 at − 1.4 V. Density functional theory (DFT) calculations show that the interface of Cu 0 /Cu + facilitates C C coupling to form C 2+ products, while inhibits CO 2 conversion to C 1 products.
研究领域:
电化学
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催化
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材料科学
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能量转换
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 2
·1218-1232
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IF 11.9
Zi-Yang Zhang,Hao Tian,Han Jiao,Xin Wang,Lei Bian,Yuan Liu,Nithima Khaorapapong,Yusuke Yamauchi,Zhong-Li Wang
The electrochemical CO2 reduction reaction (CO2RR) for high value-added multi-carbon product (C2+) production over copper oxide-based catalysts is an important way to realize the carbon cycle. However, developing effective reaction interfaces and microenvironments to improve the Faraday efficiency (FE) and current density of C2+ remains a major challenge. Herein, we construct Cu0–Cu+–NH2 composite interfaces with the assistance of SiO2. Using Cu2O nanoparticles as a model catalyst, a layer of porous SiO2 is first coated on the surface of the particles, and then, a silane coupling agent containing –NH2 is bonded on the surface of SiO2. The strong interaction between SiO2 and Cu2O at the interface induces the oxidation effect of low valent Cu, and even under the CO2RR, part of Cu+ is reduced to Cu0 and part of Cu+ still maintains positive valence, forming the interface of Cu0–Cu+. SiO2 also acts as a bridge between copper species and –NH2 to create a Cu catalyst–NH2 group interface. With the help of the synergistic effect of the composite interfaces, the optimized Cu2O@SiO2–NH2 catalyst achieves a FE of 81.2% for C2+ products with a current density of 292 mA cm−2 at −1.7 V versus a reversible hydrogen electrode. In situ Raman and attenuate total reflectance-infrared absorption spectroscopy spectra show that the interaction between surface –NH2 and CO2 molecules enhances the adsorption and activation process of CO2 and promotes the formation of CO intermediates (*CO). On the Cu0–Cu+ interface, the C–C coupling process between *CO is accelerated, and the two interfaces synergistically promote the generation of C2+ products. This work provides a new strategy for constructing composite interfaces to improve the CO2RR to C2+ products.
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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可持续能源
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DOI
高影响因子
ACS Catalysis
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2024
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IF 11.3
Long Cheng,Rong Wang,Wenzhe Si,Yanxi Deng,Junhua Li,Yue Peng
Cu-based catalysts leveraging Cu+/Cu0 active sites have emerged as pivotal for synthesizing essential hydrocarbons and alcohols in electrochemical CO2 reduction, such as ethylene and ethanol (C2 products). However, the dynamic reduction of Cu+ to Cu0 during electroreduction leads to site instability, resulting in diminished efficiency for CO2 conversion to C2 products. Herein, we introduced Si into CuO by the selective dissolution method, engendering Cu–O–Si units to stabilize the Cu+/Cu0 sites. The catalyst manifested good activity in CO2 electroreduction with an elevated Faradaic efficiency for C2 products reaching 81.9% at −100 mA/cm2. After ten cycles of electrochemical testing, the Cu+/Cu0 sites and performance exhibited no signs of degradation. The Si incorporation significantly improved the hybridization of O 2p and Cu 3d orbitals, thereby reinforcing the Cu–O bonds and stabilizing the Cu+/Cu0 sites, which was critical in promoting C–C coupling via decreasing the energy barriers for *OCCO formation and enhancing C2 product selection. The active Cu+ cations with unsaturated coordination contributed to the reaction stabilization, thereby improving the preservation of Cu2O metastable state.
研究领域:
电化学
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催化
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材料科学
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能源转化
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DOI
高影响因子
GREEN CHEMISTRY
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2025
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IF 9.2
Yahui Jiang,Haichuan He,Dan Xia,Hongwei Zhang,Shirui Tan,Li Luo,Yifan Kong,Liu Deng,You-Nian Liu
Cu-based catalysts are widely employed in the electrocatalytic CO2 reduction reaction (CO2RR) toward multi-carbon (C2+) products due to their unique electronic structures. However, Cu-based catalysts are prone to reconstruction under working conditions. Self-reduction and undesirable reconstruction have limited the activity and selectivity of these catalysts. Understanding their reconstruction behavior is crucial for elucidating reaction mechanisms and rationally designing catalysts. In this study, Br-doped Cu-base catalysts were employed to investigate the influence of dopants on catalyst surface reconstruction during CO2RR. Characterizations confirmed that during CO2RR, partial Br− leached from the precursor, while residual bromide ions in the Cu matrix created a bromine-rich environment on the catalyst surface, stabilizing Cu0/Cu+ active sites. The reconstructed catalyst exhibited superior selectivity for C2+ products and higher current density. In situ characterization and theoretical calculations demonstrated that the interaction between Br and Cu atoms suppressed complete Cu reduction. Furthermore, the asymmetric coupling pathway via *CO and *CHO intermediates dominated C2+ product formation, with significantly reduced Gibbs free energy of key intermediates compared to undoped CuO. Notably, halogen doping was validated as a universal strategy—Cu–Cl and Cu–F catalysts similarly enhanced C2+ production while exhibiting analogous reconstruction behavior. This study provided deep insights into catalyst surface reconstruction and offered effective strategies for designing high-performance catalysts for CO2RR.
研究领域:
电化学
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催化
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材料科学
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环境化学
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能量转换
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表面科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zesheng Deng,Songchang Hu,Jiahui Ji,Shiqun Wu,Haijiao Xie,Mingyang Xing,Jinlong Zhang
Cu is widely used to prepare high-value products in photocatalytic CO 2 reduction reaction (CO2PR). The valence state of transition metals usually has a great impact on the catalytic process. However, the research on Cu valence in CO2PR is lack for its complex valence change. In current work, Cu x /P25 with stable Cu valence composition in CO2PR is prepared. The results show that Cu is composed of Cu 0 and Cu 2 O, and their proportions change regularly as Cu loading changing, which are linearly related to the selectivity of the corresponding products of CO2PR. Combined with thermodynamic and kinetic analysis, the CO adsorption and activation on the surface of Cu 0 and Cu 2 O are considered to be the key to determine the product of CO2PR, which is further confirmed by DFT calculation. Cu 0 and Cu 2 O are proved to be active site of producing CH 4 and CO, respectively. In this case, a reference for the study of highly selectivity Cu based photocatalysts is provided.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）