INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Haihong Wang,Huiyan Ma,Yan Li,Lin Cheng,Jucai Yang,Juming Liu
Efficient, low-cost, and easily scalable wide-spectral-responsive TiO2 photocatalysts are still extremely desired in driving photocatalytic degradation toward practical applications. In this work, a modified TiO2 with a narrow band gap and low valence band (VB) (CC-OV-TiO2) was successfully synthesized based on a facile sol–gel and low-temperature carbonization process, which can be used for the photocatalytic degradation and mineralization of a wide range of phenols. The results show that the interstitial doping of carbonates and the modification of surface oxygen vacancy (OV) defects together contribute to the formation of the VB tail states, which substantially narrow the band gap of TiO2 and widen the photoresponse range. Meanwhile, the carboxylated carbon species induce a substantial downward shift of the VB edge through coordination of the electron-withdrawing carboxyl groups, which further enhances the oxidation ability of the photogenerated holes. Accordingly, CC-OV-TiO2 with a narrow band gap and low VB exhibits superior and stable photocatalytic performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Caizhi Lv,Pengchong Jiao,Hui Xin,Lan Wu,Gangfeng Ouyang,Xiandeng Hou
Insulator hydroxyapatite (HAp) was chosen as a candidate to construct full-spectrum photocatalyst. Glucose as a functional precursor was incorporated into HAp by coprecipitated method, and the glucose-modified HAp was then calcined under nitrogen atmosphere. With the loss of OH - group in HAp and the decomposition of glucose during the calcination, oxygen vacancies (OVs) for regulating the band gap, graphitic carbon (GC) as a good electron acceptor, and a channel for rapid carrier separation via the C-O-Ca forming between OV-HAp and GC can be simultaneously achieved. The as-prepared OV-HAp/GC displayed full-spectrum response and rapid separation of carriers. Moreover, it showed high degradation performance for 2, 4-dichlorophenol (2, 4-DCP), phenol, and tetracycline under visible, NIR, and full-spectrum. This strategy is not only facile, but also exhibits a certain universality. This work opens a new window for full-spectrum photocatalysts construction based on insulators, and large-scale production for practical use can be expected.
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FOOD AND AGRICULTURAL IMMUNOLOGY
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2023
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IF 3
Jiannan Chen,Xiuhua Xia,Peizhen Li,Hang Yu,Yunfei Xie,Yahui Guo,Weirong Yao,He Qian,Yuliang Cheng
As a type of environmentally deleterious compound, 4-nitrophenol (4-NP) has become a global concern due to its extreme toxicity to aquatic organisms and humans. Herein, we used naturally available crayfish shells as precursors to prepare a new type of carbon dots (CDs) by the hydrothermal method. The as-synthesized CDs exhibited strong blue fluorescence emission which can be sensitively quenched by 4-NP through the static quenching effect because of the formation of a ground state complex between CDs and 4-NP. Accordingly, a facile and rapid fluorescence sensor was developed to detect 4-NP from 0 μM to 50 μM with a limit of detection (LOD) of 0.16 μM. Furthermore, the proposed sensor was successfully applied for the detection of 4-NP in fresh crayfish meat and aquatic water samples.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jun Zhang,Chunyuan Wang,Shiyu Lu,Shuyue Liu,Pingjuan Liang,Huan Yi,Mengjie Li,Meng Jin,Rong Wang,Guangming Jiang
Enhancing the enrichment behavior of low-concentration chlorinated organic pollutants remains a significant challenge in electrocatalytic hydrodechlorination (EHDC) technology. Metal-loaded hollow nanoarchitecture has emerged as a promising nanoreactor to improve reaction enrichment behavior because of its tailorable microenvironments and electronic properties. Herein, a structural engineering strategy is developed to synthesize yolk-shell structured TiN spheres supported Pd nanoreactors (Pd/YS-TiN) with confined mesoscopic spaces. Characterization by multiple techniques reveals that the yolk-shell structure of YS-TiN, with high specific surface area (139.0 m 2 /g) and appropriately mesoporosity (6.9 nm), exposes numerous Pd nanoparticles (∼4.0 nm) on outer/inner surface of the shell and yolk-core solid sphere, ensuring an efficient utilization of active sites for enhancing the 2,4-DCP detoxification. Consequently, the structurally optimized Pd/YS-TiN nanoreactor consistently displays maximum reaction kinetics, dechlorination degree, faradaic current density, H* utilization and product selectivity, surpassing hollow TiN-supported Pd and Pd/C catalysts. The super EHDC performance of 91.8 % 2,4-DCP conversion, a specific activity of 1.68 min −1 mol Pd −1 , and a mass activity of 6.06 min −1 g Pd −1 is obtained at −0.85 V and 180 min, outperforming most reported catalysts. Combining experimental and density functional theory results, the exceptional reaction enrichment behavior of Pd/YS-TiN originates from (1) alleviating the overstrong adsorption of product phenol through strong metal-support interactions and (2) enhancing mass transport efficiency facilitated by the local concentration gradient and mesoporous shell. This study elucidates how metal-support interactions and mass transport synergistically enhance reaction enrichment behavior, showcasing potential benefits in environmental remediation applications.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yuxin Zhou,Minghua Liu,Yuancai Lv,Hong Guo,Yifan Liu,Xiaoxia Ye,Yongqian Shi
In this work, a lignin phenolic carbon foam (LCF) with preferable smoke suppression performance was fabricated by substitute 10 wt.% and 30 wt.% phenol with modified lignin in the traditional process. The result showed that the LCF 600 s (LCFs carbonized at 600℃) with different lignin percentages showed better smoke suppression performance than the traditional phenolic carbon foam (CF 600 ). The peak smoke production rate (pSPR) and total smoke release (TSR) of LCF 600 s decreased by 6.90%∼48.28% and 80.91%∼96.28%, and the peak CO production rate and CO yield decreased by 41.17%∼70.59% and 53.80%∼77.79%, respectively. Besides, LCF 1-10-600 and LCF 2-30-600 displayed the best smoke suppression performance (0020, 0.0015 m 2 /s of pSPR and 0.61, 2.76 m 2 /m 2 of TSR, respectively). Since the introduced modified lignin significantly increased the amount of benzene rings in the forms, the degree of graphitization of the resulted carbon foams greatly improved, leading to better smoke suppression performance. Furthermore, the added lignin facilitated the preservation of the carbon layer, resulting in reducing smoke production consequently.
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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.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Weiwei Wang,Jin Jiang,Qinglong An,Rui Shi,Shuyang Shao,Zhi Wang
Due to its outstanding properties, benzoxazine resin is widely used in the manufacturing of machinery, aerospace, and electrical products. However, once polybenzoxazine and its composites reach the end of their useful lives, their three-dimensional network structure and persistent cross-linking after curing pose challenges for degrading. To address this issue, our study focuses on incorporating 2,3-dihydrofuran (DHF)-containing cleavable bonds into the cross-linked network of benzoxazine (PH-5n2m) containing the structure of norbornene by ring-opening metathesis polymerization (ROMP). Due to the unique chemical structure of norbornene and the flexibility of the DHF chain segment, poly(PH-5n2m/DHF-x) exhibits remarkable thermal stability and improved toughness compared to poly(PH-5n2m). Additionally, under weak acid conditions, the PH-5n2m/DHF-50/CF composite can degrade fully in less than 10 h, facilitating the nondestructive recycling of the carbon fiber. This work presents a novel approach to the development of thermosetting resins with high thermal stability, improved toughness properties, and degradability, offering promising prospects for sustainable materials in various industries.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Qi-Xin Wei,Ai-Yong Zhang,Zedong Yang,Song Hu,De-Jin Wang,Chi Zhang,Chang Liu,Rui Liu
Solid catalyst plays the governing role in the heterogeneous Fenton-like catalysis for water purification . In this work, the Co(II)-doped C 3 N 4 (Co/C 3 N 4 ) was prepared and further thermally exfoliated in different atmosphere for the three-dimensional layered configuration. The morphological and structural properties as well as surface chemistry of Co/C 3 N 4 before and after thermal exfoliation were elucidated in comparison. The oxygen-exfoliated Co/C 3 N 4 (O-Co/C 3 N 4 ) exhibited accessible metal exposure and synergistic pollutant adsorption stemmed from three-dimensional layered configuration with ordered porous configuration, oriented lamellar structure and increased surface area. Moreover, an excellent Fenton-like reactivity and stability was measured for PMS activation and pollutant degradation , and the comparative performance before and after oxygen exfoliation as well as with typical metal-based catalysts were investigated in details. The impacts of testing conditions and water matrices were elucidated to estimate environmental potential. Based on radical identifying and inhibiting tests and electrochemical measurements, the non-radical reaction pathway from mediated electron transfer (MET) played the key role with much reduced matrix effects and satisfactory catalytic selectivity . This work provides a new chance to save transition-metal consumption and refine Fenton-like reactivity in C 3 N 4 -based catalysts for superior environmental remediation.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Xiangfen Xue,Mingjie Wei,Jing Yuan,Xinyu Huang,Qinghua Cao,Changkun Xia,Xiangheng Niu,Xiulian Yin
A convenient, fast, low-cost detection and discrimination method is demanded for environmental monitoring but still it remains more technological challenges. Herein, we demonstrate that the inner filter effect (IFE), in combination with three-dimensional fluorescence spectroscopy, can offer a virtual sensor array (VSA) as a proper solution. And with the aid of pattern recognition techniques, it is feasible to recognize compounds with structural similarities economically and effectively. In this study, with the help of visual clustering plots of principal component analysis (PCA), a prediction model based on hierarchical strategy was made using support vector machine (SVM) method for the qualitative profiling of aromatic pollutants. The VSA was constructed by a single metal–organic framework (MOF) recognition unit (MOF-74 (Zn)) with the excitation wavelength as external regulatory factors. Pattern characteristics of four aromatics with very similar structures (phenylamine, chlorobenzene, nitrobenzene, and phenol), both single analyte and binary mixtures, were acquired. The primary constituents of multi-dimensional spectral signals were subsequently extracted and fed into a vector machine to construct a prediction model through 10-fold cross-validation optimization, resulting in a classification accuracy of 100% for single analytes and 96% for mixtures. Quantitative research has shown that, except for chlorobenzene, all three other analytes can be predicted in concentration within an acceptable error range, and the mixture can be predicted proportionally. Moreover, the VSA can be used to distinguish these pollutants in tap and river water also. We propose for the first time a new tack for the construction of VSA in a general manner, namely using three-dimensional full range fluorescence scanning for IFE based sensing to get multiple times of information resulting from different weak interaction between analyte and sensor for decision-making.
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Separations
·
2023
·Vol. 10
·期 10
·523
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IF 2.6
Xiangfen Cui,Jingmei Liao,Huaying Liu,Wei Tang,Cheng Tie,Senlin Tian,Yingjie Li
The presence of organic pollutants in wastewater remains a prominent environmental concern due to the related ecological and health hazards. In response, this study employs an adsorptive methodology to address the removal of phenol and catechol, utilizing an organo-bentonite material modified with a pH-responsive switchable surfactant, dodecyldimethylamine oxide (C12DAO). The synthesized organo-bentonite (C12DAO-Bt) manifests commendable thermostability resulting from thermogravimetric analyses. The adsorption capacities of C12DAO-Bt concerning phenol and catechol intensify with the augmentation of the C12DAO/bentonite mass ratio. The utmost adsorption capacities of 150C12DAO-Bt, deduced through a pseudo-second-order kinetic model, stand at 5.72 mg·g−1for phenol and 5.55 mg·g−1for catechol, respectively. Subject to modification by a pH-responsive surfactant, conditions leaning towards weakly acidic and neutral conditions (pH = 6~7) are conducive to the adsorption of phenolic compounds. Conversely, alkaline conditions (pH = 8~9) facilitate the dissociation of adsorbates from adsorbents. The augmentation of cationic strength within the examined scope incites the adsorption procedure while impeding the desorption efficacy. In the case of cationic species with comparable ionic strengths, Na+exhibited a superior effect on the adsorption–desorption dynamics of phenol, while Ca2+exerts a more pronounced effect on those of catechol. Moreover, even following five consecutive acid–base regulation cycles, C12DAO-Bt retains a relatively high adsorption capacity and desorption efficacy, which underscores its exceptional regenerative capacity for removing phenolic compounds from wastewater.Keywords:pH-responsive surfactants;organic bentonite;reversible adsorption;phenolic pollutants;wastewater
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Tianbo Zhou,Xueshuai Wang,Yi Liu,Liuchun Zheng
The conventional direct esterification and polycondensation is difficult to obtain kilogram scale of poly(butylene succinate) (PBS) ionomers with both high molecular weight and high ionic group content. Therefore, the investigation of relationship between the content of ion group and performance (such as mechanical properties) is impossible. In this work, the preparation of PBS ionomers with high molecular weight and high ion group content was achieved by transesterification method using sodium dimethyl isophthalate-5-sulfonate (SIPM) as the ionic monomer, and the polycondensation time decreased significantly with the increase of SIPM content. The mechanism of reducing the polycondensation time of PBS prepared by transesterification is proposed. The tensile strength, flexural strength and impact strength of PBS ionomers increased significantly with increasing SIPM content. At high ion group content, the formed multiplets-clusters among ion groups, which act as reversible physical crosslinking points and nano-fillers, substantially improved the mechanical properties. The tensile strength, flexural strength and impact strength improved and reached to 50.1 MPa, 40.9 MPa and 13.1 kJ/m 2 at high ion group content from 34.2 MPa, 24.1 MPa and 5.8 kJ/m 2 for PBS, respectively. It showed a totally opposite trend from the previous research. In addition, the hydrophilicity and processing properties of PBS ionomers improved significantly with the increase of the ion group content, and the contact angle reduced to 41.1° after the introduction of ions.
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FUEL PROCESSING TECHNOLOGY
·
2023
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IF 7.5
Fa-Peng Wu,Le-Le Qiu,Yun-Peng Zhao,Zong-Pin Fu,Jian Xiao,Jian Li,Fang-Jing Liu,Jing Liang,Jing-Pei Cao
Catalytic hydrodeoxygenation (HDO) of phenolic compounds is a promising strategy for bio-oil upgradation to produce high-value chemicals and fuels. Herein, a series of NiFeAlO x catalysts prepared by a co-precipitation method were applied in HDO of guaiacol as a typical model compound. The characterization results revealed that the catalyst with Ni/Fe/Al ratio of 3/0.5/2.5 possessed developed textural properties, small metal particles, abundant oxygen vacancies and acid sites. HDO of guaiacol occurred in two pathways with different hydrogen sources : the direct hydrogenation of benzene ring to 2-methoxycyclohexanone and the further hydrogenolysis and dehydration of intermediates to cyclohexane at 260 °C in n -hexane under H 2 for 6 h, while demethoxylation affording phenol followed by hydrogenation of phenol to cyclohexanol at 220 °C in isopropanol under N 2 for 2 h. The different product composition results from the type of reactive H species, where active hydrogen species are hydrogen radicals using H 2 as the hydrogen source and hydrogen ions with opposite charges using isopropanol as the H-donor solvent, respectively. The Ni 3 Fe 0.5 Al 2.5 O x catalyst maintained good performance after five recycle experiments with a slight decrease in the conversion of guaiacol. Moreover, the catalyst showed excellent universality for selective HDO of other phenolic compounds to cycloalkanes or cycloalkanols.
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