SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Na Liu,Yinhui Li,Minggu Zhang,Naiju Che,Xianliang Song,Yanli Liu,Chengliang Li
As the substitutes of legacy long-chain per-/polyfluoroalkyl substances (PFASs), short-chain PFASs have been widely detected in the environment. Compared to long-chain PFASs, short-chain PFASs have smaller molecules and are more hydrophilic. Therefore, they are more likely to experience long-distance transport and pose lasting environmental impacts. In this study, Fe-doped (R-Fe) and Cu-doped biochars (R-Cu) were prepared using reed straw biochar (R). The results showed that the PFBA and PFPeA sorption capacities of R-Fe were 25.81 and 43.59 mg g −1 , 1.65 and 1.55 times higher than those of R, respectively. The PFBA and PFPeA sorption capacities of R-Cu were 19.34 and 33.69 mg g −1 , 1.24 and 1.20 times higher than those of R, respectively. In addition, R, R-Fe, and R-Cu exhibited higher PFBA and PFPeA sorption capacities than the biochars previously reported. The excellent PFAS sorption performances of the biochars were attributed to the highly porous structure of R, which provided rich adsorption sites. Ion-pair sorption, pore filling, electrostatic interaction between the Fe/Cu and cationic groups on biochar and the anionic groups of PFASs, and hydrophobic interaction between the hydrophobic surface of biochar and the fluorinated tails of PFASs were the underlying sorption mechanisms. The biochars presented high removal rates (>86 %) of multiple PFASs (∑PFAS: 350 μg L −1 ) from synthetic wastewaters, including legacy and emerging PFASs of different chain lengths and with different functional groups. The biochars reported in this study are promising candidate adsorbents for treating waters contaminated with short-chain PFASs.
CAS / MDL:
研究领域:
环境科学
·
污染控制
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Peng Wang,Wei Nong,Yan Li,Hao Cui,Chengxin Wang
Although the electrochemical nitrogen reduction reaction (NRR) is regarded as a promising alternative to the Haber–Bosch process, it still suffers from the poor activity and low selectivity. Herein, we propose a powerful strategy to simultaneously boost the activity and selectivity by introducing strain engineering into the design of NRR electrocatalysts. The strain-engineered electrocatalysts consisted of monodisperse CuAu@Cu core-shell nanoparticles with controllable Cu skin via one-pot solvothermal process. Among them, electrocatalysts with about 2 layers of atomic Cu skin (CuAu@2LCS) achieve the highest NH 3 yield rate (33.9 μg NH3 h −1 mg cat. −1 ) and Faradic efficiency (24.1 %) at –0.2 V vs. RHE in 0.1 M HCl. Density functional theory (DFT) calculations reveal that owing to the unique structure of bimetallic alloys with the ultra-thin Cu skins, tensile strain and favorable ligand effect work together and tune the surface electronic structure of electrocatalysts, which not only strengthen N 2 affinity but also suppress the competitive HER process.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
CHEMOSPHERE
·
2023
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IF 8.8
Huiwang Dai,Jingyi Zhu,Fanxu Meng,Daohui Lin,Wenjun Zhou,Dingjiang Chen,Ming Zhang,Qingqing Wang
In this study, Cu hybridization coupling oxygen defect engineering was adopted to synthesis of CuNiFe layered double oxides (CuNiFe-LDOs) in peroxymonosulfate (PMS) activation for degradation of methyl 4-hydroxybenzoate. The morphology and crystal structure of CuNiFe-LDOs was characterized in detail, which exhibited regular layered-structure at a Cu:Ni doping ratio of 1:1 and annealing temperature of 400 °C, and presented the crystal of Cu x O@Fe 3 O 4 –NiO. Besides, the X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) results demonstrated that abundant oxygen vacancies (OVs) and low oxidation state Cu species were composed in CuNiFe-LDOs400. The Cu 1·5 Ni 1·5 Fe 1 -LDOs400/PMS system showed excellent catalytic performance toward the degradation of butyl 4-hydroxybenzoate (BuP), and resistant to the effect of pH value and background inorganic anions. Based on quenching experiments and EPR measurements, singlet oxygen ( 1 O 2 ) was identified as the dominant active species during the heterogeneous catalytic process, which was generated by the synergistic interaction between OVs-Cu(I) site and PMS . In this process, the electron-drawing property of OVs promoted the adsorption of PMS molecule on Cu(I) site, followed by the accumulation of electron and cleavage of O–O bond to generate intermediate oxygen radical species, which donated one electron to eventually generate singlet oxygen.
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
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Jie Chen,Chenyi Zheng,Qiang Wang,Zhipeng Xu,Kui Meng
Many innovations have been made in the morphology and preparation methods of copper–silver core–shell nanomaterials (Cu@AgNMs). The most commonly used method for preparing Cu@AgNMs is to perform a replacement reaction by adding a complexing agent, but there is no universally accepted method to select a complexing agent. This study found that the best complexing agent for preparing Cu@AgNMs is a short-chain complexing agent containing hydrophilic groups through the role of different complexing agents in the synthesis of the material, and the higher the stability of the short-chain hydrophilic complexing agent, the better the integrity of the resulting silver layer. This study clarifies the mechanism of different complexing agents in the synthesis of Cu@AgNSs, provides a reliable reference for the convenient preparation of Cu@AgNMs, and helps us to understand the influence of complexing agents on the silvering effect of the replacement process, thereby promoting the widespread application of a complex-replacement technology.
研究领域:
材料科学
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纳米技术
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化学工程
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Liang Zhu,Yang Liu,Yanhui Gao,Ningxujin Ding,Danyu Wang,Liuliu Long,Beibei Wang,Junyu Lang,Evgeny I. Vovk,Yong Yang
The hydrogen dissociation and spillover mechanism on oxide-supported Cu catalysts play a pivotal role in the hydrogenation of carbon dioxide to methanol. This study investigates the hydrogen spillover mechanism on Cu/CeO2 catalysts using in situ spectral characterization under high-pressure reaction conditions and density functional theory (DFT) simulations. The research confirms that the Cu sites serve as the initial dissociation points for the hydrogen molecules. The chemically adsorbed hydrogen (H*) then spills over onto the CeO2 support and interacts with the lattice oxygen to form special hydroxyl groups, while simultaneously reducing the surrounding Ce4+ to form Ce3+. Interestingly, the temperature-programmed desorption (TPD) results found that heating the hydroxyl-containing surface mainly reverses H2 dissociation by desorbing H2 instead of forming H2O, while no significant vacancy formation was detected. The DFT calculation identified a subsurface pathway favoring hydrogen migration, which explained the dominating H2 in the TPD products. A chemical loop study after CO2/H2 cofeeding on the catalyst reveals that hydrogen spillover facilitates the highly reduced surface serving as the active centers, enabling a secondary methanol synthesis in a vacuum. This study provides a model of the formation and desorption pathways of hydrogen species on Cu/CeO2 catalysts and illustrates the key role of the hydrogen spillover mechanism in promoting the CO2 hydrogenation to methanol reaction through important experimental analysis.
研究领域:
催化化学
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材料科学
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理论计算化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guangping Lei,Guojun Xi,Zihan Liu,Qibin Li,Huiyuan Cheng,Hantao Liu
Efficient capture and separation of CO 2 from flue gas and natural gas are highly promising to reduce carbon emissions and promote fuel calorific value. Here, a novel adsorbent (FeTPPs@Cu-BTC) for CO 2 separation was synthesized by encapsulating 5, 10, 15, 20-tetrakis (4-sulfonatophenyl) porphyrinato iron (III) chloride (FeTPPs) into the cages of Cu-BTC through an in-situ packaging strategy. Such strategy efficiently overcomes the shortcoming of pore clogging and leaching induced by incorporating guest molecules through the wet impregnation method. Meanwhile, more tunable micropores and extra affinity sites for CO 2 adsorption were created after encapsulation of FeTPPs, which preferably enhanced the CO 2 uptakes of FeTPPs@Cu-BTC under low pressures and promoted the separation performances for CO 2 /N 2 (15:85, v/v) and CO 2 /CH 4 (50:50, v/v) mixtures. The corresponding selectivity of FeTPPs@Cu-BTC calculated by ideal adsorbed solution theory (IAST) respectively increase to 57.7 and 14.0 from 36.0 and 10.8 of the pristine Cu-BTC at 273 K and 100 kPa, which also exceeds most reported adsorbents. Grand Canonical Monte Carlo (GCMC) simulations further elucidated that extra interaction with CO 2 and ‘sieve effect’ for N 2 or CH 4 after FeTPPs encapsulation immediately boost CO 2 uptakes and separation performance of FeTPPs@Cu-BTC. This study provides a new design idea for the development of new adsorbent 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
Small
·
2023
·Vol. 19
·期 40
·2303099
·
IF 13.3
Zi Yang,Deguang Ji,Zhi Li,Zidong He,Yang Hu,Jie Yin,Yichao Hou,Pinxian Xi,Chun-Hua Yan
Copper-based electrocatalysts effectively produce multicarbon (C 2+ ) compounds during the electrochemical CO 2 reduction (CO 2 RR). However, big challenges still remain because of the chemically unstable active sites. Here, cerium is used as a self-sacrificing agent to stabilize the Cu + of CuS, due to the facile Ce 3+ /Ce 4+ redox. CeO 2 -modified CuS nanoplates achieve high ethanol selectivity, with FE up to 54% and FE C2+ ≈ 75% in a flow cell. Moreover, in situ Raman spectroscopy and in situ Fourier-transform infrared spectroscopy indicate that the stable Cu + species promote C C coupling step under CO 2 RR. Density functional theory calculations further reveal that the stronger * CO adsorption and lower C C coupling energy, which is conducive to the selective generation of ethanol products. This work provides a facile strategy to convert CO 2 into ethanol by retaining Cu + species.
研究领域:
材料科学
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催化化学
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能源转化
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产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Ji Yaxiong,Lin Shuang,Xu Guihong,Chen Tianen,Gong Jianchao,Meng Fanbin,Wang Yuanhao
Abstract Catalytic conversion of CO 2 to methanol with H 2 from renewable energy has attracted increasing interest as a promising strategy for reducing excessive CO 2 emissions. However, the performance of reported various catalysts still suffers from low methanol yield with a passable CO 2 conversion. In this work, Cu–ZnO–La 2 O 3 interfaces are constructed with various La 2 O 3 mole ratio. Compared to Cu/ZnO, the optimized catalyst (i.e., Cu 0.6 Zn 0.2 La 0.4 ) exhibits a much higher mass-specific methanol formation rate (159.3 g MeOH /kg cat /h) at 240 °C and 3 MPa. A series of ex-situ and in-situ characterizations, such as X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), N 2 O titration measurements, and in-situ diffuse reflectance Fourier transform infrared spectroscopy ( in-situ DRIFTS) study, are used to investigate its structure and mechanism study. The dispersion of Cu over Cu/ZnO/La 2 O 3 catalyst is significantly enhanced, forming more Cu–ZnO–La 2 O 3 interfaces. LaO x species favor CO 2 activation and generate more carbon intermediates species for CO 2 hydrogenation. Furthermore, more Cu + is bonded, which stabilizes the key intermediate, inhibits its desorption, and facilitates its further hydrogenation to methanol. This work is expected to offer an effective strategy to develop new catalysts with high performance for CO 2 hydrogenation to methanol. Graphical Abstract
研究领域:
催化化学
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能源化学
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材料科学
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DOI
高影响因子
RENEWABLE ENERGY
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2020
·
IF 6.274
Yunwu Zheng,Jida Wang,Can Liu,Yi Lu,Xu Lin,Wenbin Li,Zhifeng Zheng
To eliminate the problematic need for liquid phase, high temperature, and high pressure, as well as the excessive consumption of hydrogen and production of aromatic hydrocarbons, associated with traditional aviation oil preparation processes, Ni–Cu bimetallic catalysts were synthesized and evaluated for ex situ catalytic pyrolysis vapor upgrading of oleic acid under a N 2 atmosphere. The effects of catalyst support (AC, Al 2 O 3 , ZrO 2 , HZSM-5, HUSY, Hβ and MCM-41), pyrolysis process parameters (pyrolysis temperature, catalytic temperature and amount of oleic acid injected), and the mixing ratio of modified metals (Ni:Cu = 0:1,2,1:1,1:2,1:0) on the catalytic conversion of oleic acid to high-quality chemicals were studied. The catalysts were characterized by XRD , BET and NH 3 -TPD. Modified bimetallic catalysts show great potential for green diesel production without the use of H 2 feed. The abundance of Brønsted acid sites favors HDO routes (such as HZSM-5, HUSY, Hβ and MCM-41), while Lewis acid sites (such as ZrO 2 and Al 2 O 3 ) favor hydrogenation and decarbonylation reactions. The addition of Cu enhances the reducibility of Ni and inhibits the cracking reaction and deactivation caused by coke. The addition of Ni effectively promotes the conversion of oleic acid, accelerates the fracture of C–C and effectively improves the production of hydrocarbons. The highest conversion was 100% with 85.68% selectivity towards hydrocarbons under pyrolysis at 450 °C, a catalytic temperature of 500 °C, and a feed quantity of oleic acid of 0.25 ml/min using Ni–2Cu/MCM-41 catalysts, and the oxygen removal efficiency and selectivity of C17 hydrocarbon were the highest (85.68% and 26.77%, respectively). The main products were olefins . In addition, the regenerated catalyst had good stability and could be used for at least 3 reaction cycles without observation of significant deactivation.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 6
·4443-4457
·
IF 4.6
Junqi Zhang,Yongwang Li,Zhiwei Zhang,Zheng Wang,Jiaxing Zhang,Shuai Liu,Yang Qin,Bingxin Zhu,Tongxue Zhang,Hongyu Wang,Fumin Wang,Xubin Zhang
The development of simple, efficient and economical catalysts for the hydrogenation of biomass to produce high value-added chemicals is of great significance in solving the energy crisis. In this work, a series of non-precious metal catalysts (Cu–Al2O3–ZnO) with different defect sites were prepared by etching Devarda's alloy. Under optimized mild reaction conditions, the furfural conversion and furfuryl alcohol selectivity are both greater than 99.0%, and the catalyst has good reusability. Characterisation and experiments were used to investigate the activate species for hydrogenation reaction. It can be proved that the low-valent Cu species in the Cu–Al2O3–ZnO catalysts play an important role as adsorption and dissociation sites for H2. Different etching degrees and sample reduction temperatures of the alloy can be used to adjust the content of acidic sites such as Al2O3 and CuO, which have appropriate adsorption properties for furfural. ZnO promotes the dispersion of the Cu species and enhances the accessibility of the active sites. The etching method achieves the interaction between species to further enhance the stability and activity of the catalyst. The catalytic performance of the catalyst is very competitive and this study provides a new method for the efficient hydrogenation of furfural to furfuryl alcohol.
研究领域:
化学工程
·
可再生能源
·
催化科学
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产品关联
DOI
PubMed
高影响因子
CARBON
·
2022
·
IF 11.307
Jing Chen,Ying Chen,Shuying Li,Jiao Yang,Jianbin Dong,Xiaoquan Lu
Tyrosine is the precursor of some neurotransmitters such as thyroxine and dopamine. It has the effect of regulating emotions and stimulating the nervous system. Changes in tyrosine levels in the human body are associated with certain diseases. Therefore, it is very necessary to prepare a new type of tyrosine sensor. In this work, an enzyme-free electrochemical sensor based on MXene/CNTs/CuMOF composite was developed for the detection of tyrosine. Embedding carbon nanotubes (CNTs) into MXene effectively prevented the aggregation of MXene sheets. Further modification of MXene/CNTs materials with CuMOF octahedral particles with porous structure can improve the porosity and catalytic capability of the composites. Under the optimal detection conditions, the prepared sensor has good linearity in the detection of tyrosine within range 0.53 μM–232.46 μM with a limit of detection (LOD) of 0.19 μM. The stability and selectivity of the sensor is high, and can be used to detect tyrosine in human serum.
研究领域:
生物医学工程
·
分析化学
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产品关联
DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2020
·
IF 4.333
Xin Zong,Jie Zhang,Jinqiu Zhang,Wen Luo,Andreas Züttel,Yueping Xiong
The electrochemical reduction of carbon dioxide (CO 2 RR) has attracted enormous interest because of the energy crisis and climate change; however, more efficient catalysts are required for practical applications. Herein, we present electrospinning as a facile strategy to synthesize a three-dimensional network of carbon nanofibers embedded with Cu and CeO x nanoparticles (Cu/CeO x @CNFs) as a CO 2 RR catalyst. The Cu–CeO x interface produced using this method offers synergistic geometric and electronic effects which optimize the adsorption strength of reaction intermediates for the electroreduction of CO 2 to CO. In a flow cell configuration, a current density of 100 mA cm −2 and a CO faradaic efficiency of 59.2% can be obtained at −0.60 V vs. RHE.
研究领域:
电化学
·
材料科学
·
催化
·
纳米技术
·
能源转换
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）