INDUSTRIAL CROPS AND PRODUCTS
·
2026
·
IF 6.4
Wendi Fang,Naixin Kang,Le Huang,Guiying Dai,Xueting Fei,Hongxu Liang,Hongxiang Hu
The reduction and precipitation of Cr during the adsorption process has always been challenging. In this study, S and N codoped lignin-based porous carbon (SN-LPC) was prepared by hydrothermal treatment and K-intercalation activation for the removal of Cr(VI). We discovered that SN-LPC has a new mechanism underlying the adsorption–reduction–readsorption of Cr(VI): First, SN-LPC adsorbs Cr(VI) onto its surface through the hydrogen bonding of -OH and the electrostatic adsorption of N functional group protonation; second, the S and N functional groups act as electron donors to induce the rapid reduction of Cr(VI) to Cr(III). Last, the –C–OR/C N groups on the SN-LPC surface and the S and N functional groups adsorb Cr(III) again, increasing the removal of Cr(VI). DFT calculations have revealed at the molecular structure level that SN-LPC has a more active electronic nature. Doping of S and N increases the affinity of SN-LPC for chromium, which explains why it can efficiently reduce and fix Cr(VI) and adsorb Cr(III). The removal process of Cr(VI) by SN-LPC is mainly multilayer adsorption dominated by chemical adsorption, with a maximum adsorption capacity of 967.45 mg/g (pH 2, 45 °C, and an initial concentration of 800 mg/L), and the removal efficiency is much greater than that of similar activated carbon and biochar. The 2D-FTIR–COS results further elucidated the sequence of functional groups of SN-LPC in the process of reducing Cr(VI), supporting the mechanism hypothesis of adsorption–reduction–readsorption. These findings highlight the significance of sulfur and nitrogen as key groups in reduction and adsorption and provide a reference for the underlying synergistic adsorption reduction mechanism used to repair Cr(VI).
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Biochar
·
2023
·Vol. 5
·期 1
·1-20
·
IF 12.7
Yang Bowen,Dai Jiawei,Zhao Yuan,Wang Zhanchao,Wu Jingwei,Ji Caiya,Zhang Yuhu,Pu Xiao
Biochar-coupled Fe 3 O 4 @SiO 2 /TiO 2 /g-C 3 N 4 composites were successfully constructed through simple sol–gel and calcination methods. The composites efficiently removed high-concentration toxic tetracycline (TC) by means of ·OH and · \({\rm O}_2^{-}\) , whose removal rate exhibited 91.88% during 3 h, and the degradation rate constant reached up to 0.0068 min −1 . The excellent performance can be attributed to the high specific surface area, enhanced visible light response, the introduction of magnetic nanoparticles and biochars expediting charge transfer, Z-scheme heterojunction enhancing the spatial separation of photo-generate carriers and, importantly extraordinary adsorption capacity of 147.96 mg g −1 . Moreover, the composites showed the most excellent efficiency under the calcination temperature of 450 ℃, and exhibited good stability with tolerance to a wide range of pH and anions. Interestingly, a synergistic photocatalytic effect was discovered in the TC/Cr(VI) combined pollution systems, resulting in significantly improved removal of Cr(VI). Besides, the photocatalytic mechanism and degradation path of tetracycline were also elucidated. All these findings suggested the as-synthesized catalyst was an excellent photocatalyst for removal of TC/Cr(VI)-contaminated water. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Guangping Lei,Yang Lu,Zihan Liu,Yayun Zhang,Guojun Xi,Huiyuan Cheng,Wenji Rao,Xuhuan Guo
The greenhouse effect associated with excessive CO 2 emission has led to a series of environmental issues, thus developing excellent adsorbents for CO 2 capture from flue gas offers a sustainable approach. To combine the merit of multiple functional components, novel FeTPP@MIL-101(Cr) was prepared by incorporation of 5,10,15,20-tetrakis(4-methylphenyl)porphyrinato iron (III) chloride (FeTPP) into MIL-101(Cr) cages via in-situ packaging strategy. The cage-confined FeTPP can both regulate the pore structures of MIL-101(Cr) and provide additional binding sites for CO 2 adsorption. Profiting from extra interactions for CO 2 component and the “sieving effect” for N 2 component induced by incorporation of FeTPP, the discrepancy of isosteric heat for CO 2 and N 2 was largely amplified. Notably, the CO 2 /N 2 selectivity (15/85, v / v ) calculated by ideal adsorbed solution theory (IAST) increased from 17.1 (MIL-101 (Cr)) to 41.8 (FeTPP@MIL-101 (Cr) with FeTPP loading of 4.98 wt%) at 273 K, 100 kPa, which is 2.44 times larger than that of pristine MIL-101 (Cr) and also exceeds most reported adsorbents.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 29
·15760-15768
·
IF 11.9
Chunyan Xiong,Shan Xu,Xiantao Li,Tong Liu,Yuan Tan,Pei Zhao,Peng Qiu
The sluggish oxygen reduction reaction (ORR) kinetics and the fast performance degradation caused by Cr-poisoning greatly hinder the commercialisation of an LaxSr1–xCoyFe1–yO3–θ (LSCF) cathode in solid oxide fuel cells (SOFCs). Herein, a surface regulating and hetero-interface engineering method by chemical vapour deposition (CVD) was applied to construct a CeO2-coated LSCF cathode with enhanced ORR activity and durability. By controlling the CVD operating time, and the thickness of the CeO2 coating, the CeO2/LSCF heterointerface could be precisely engineered. With the optimal CVD time of 7 min, the x-LSCF cathode exhibited a minimal polarisation resistance (Rp) value of 0.11 Ω cm2 at 750 °C, which is almost one-fifth of that of an LSCF cathode (0.46 Ω cm2). Moreover, the CeO2-coated LSCF cathode exhibited a much lower degradation rate than the LSCF cathode in the long-term Cr-poisoning test. The improved ORR catalytic activity and durability of the CeO2-coated LSCF cathode were also verified in the single-cell mode. This study provides a comprehensive and novel strategy for tailoring the surface of the SOFC cathode for achieving enhanced performance and Cr-tolerance.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Hao Dong,Li Zhang,Penghui Shao,Zichao Hu,Ziwei Yao,Qingying Xiao,Dewei Li,Min Li,Liming Yang,Shenglian Luo,Xubiao Luo
Given the large amount of toxic Cr(VI) wastewater from various industries, it is urgent to take effective treatment measures. Adsorption has been regarded as highly desirable for Cr(VI) removal, but the effectiveness of most adsorbents is significantly dependent on pH value, in which precipitous performance drop and even structural collapse generally occur in strong acidic/alkaline aqueous. Thus, maintaining high adsorption performance and structural integrity over a wide pH range is challenging. To efficiently remove Cr(VI), we designed and prepared of an acid-base resistant metal-organic framework (MOF) Zr-BDPO, by introducing weak acid-base groups (-NH-, -N= and -OH) onto the ligand. Zr-BDPO achieved a maximum adsorption capacity of 555.6 mg · g −1 and retained skeletal structure at pH= 1–11. Interestingly, all these groups can generate conjugate acid-base pairs by means of H + and OH - in the external solution and then form buffer layer. The removal of Cr(VI) at a broad range of pH values primarily via hydrogen bonds between -NH- and -OH, and the oxoanion species of Cr(VI) is unusual. This strategy that insulating high concentrations of acids and bases and relying on hydrogen bonds to capture Cr(VI) oxoanions provides a new perspective for actual Cr(VI) wastewater treatment .
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高影响因子
Materials Advances
·
2022
·Vol. 3
·期 20
·7546-7558
·
IF 0
Hecheng Ma,Jianjun Liu,Yimeng Wang,Shengli Zuo,Yingchun Yu,Baoshan Li
Photocatalytic degradation has been developed as a promising strategy for environmental remediation. Black phosphorus (BP) has attracted much attention in the field of photocatalysis due to the adjustable bandgap and high carrier mobility. In this work, we constructed a flower-like BP nanosheet/P-doped BiOCl (BP/P-BiOCl) S-scheme heterostructure via a simple co-precipitation method. The physicochemical properties such as the crystallinity, morphology, chemical environment, and optical and electronic properties of the as-fabricated materials were analyzed by using different analytical techniques. SEM data indicated the successful formation of a flower-like structure of BP/P-BiOCl composites. X-Ray photoelectron spectroscopy data indicated the formation of P-doped BiOCl. X-Ray diffraction and high resolution-TEM data revealed the formation of a hierarchical BP/P-BiOCl heterostructure. The catalytic activity of the as-synthesized samples (15%-BP/P-BiOCl) was tested towards RhB degradation (96% of 20 ppm RhB solution) and Cr(VI) reduction (90% of 20 ppm Cr(VI) solution) under solar light illumination. We demonstrated the formation mechanism of a flower-like structure in which positively charged BPNs assembled with negatively charged P-BiOCl by electrostatic attraction. Furthermore, we revealed the S-scheme photocatalytic mechanism to prove the enhanced photocatalytic activity of BP/P-BiOCl composites. The photodegradation of phenol, radical species trapping experiments and charge transfer route test were performed to prove the formation of the S-scheme. This work provides a facile route for the construction of a flower-like S-scheme heterostructure photocatalyst for efficient solar light photocatalytic performance.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Xiaodan Ding,Waqas Ahmad,Muhammad Zareef,Yawen Rong,Yunlian Zhang,Jizhong Wu,Qin Ouyang,Quansheng Chen
In this study, an ultra-sensitive and selective biosensor for the detection of enrofloxacin (ENR) in complex matrices has been established. The study intelligently converges the spectral properties of core-shell upconverted nanoparticles (UCNPs) and the excellent adsorption satiating aptitudes of metal organic frameworks (MOFs). The principle was based on the fluorescence resonance energy transfer (FRET) between aptamer-modified UCNPs as the donors and MOFs MIL-101(Cr) as the effective receptors. The spectral overlap between UCNPs fluorescence emission and MIL-101(Cr) absorption generated the FRET process under the action of π-π stacking interactions. The presence of ENR induced conformational changes in the aptamer via preferential binding, resulting in a decline in the nucleobase exposure on the surface of MIL-101(Cr) and eventually in the fluorescence recovery. The fluorescence intensity (FL) was enhanced as the ENR concentration was increased. The detection limit was 0.034 ng⋅mL −1 and the linear calibration curve between logarithmic ENR concentration and FL was achieved in the range of 0.1–1000 ng⋅mL −1 . The applicability of the platform for ENR recognition was confirmed in real fish and shrimp samples and further validated by a standard HPLC technique with no significant difference (p > 0.05). The current UCNPs-MIL-101(Cr) aptasensor proposes a fast, sensitive and quantitative detection approach for ENR in aquatic products.
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JOURNAL OF COORDINATION CHEMISTRY
·
2021
·
IF 1.751
Milad Taheri
The synthesis and properties of new hybrid core-shell nanoparticles SiO2-HPW12O40@Fe3O4/EN-MIL-101(Cr) are reported. These hybrid nanomaterials were synthesized by binding of Keggin-type heteropolyacid (HPA) on diamine-activated Fe3O4 magnetic nanoparticles. The present work proposes an electroanalytical method for selective determination of losartan antihypertensive drug (LOS). Under optimal conditions, an electrochemical sensor was performed between the molecules in 0.1 M phosphate buffer (PBS) pH 6.0. Heterogeneous nanocatalysts can be easily separated from the reaction mixture using a magnet and used multiple times. The structure of the synthesized nanocatalyst was determined by various physicochemical techniques such as TEM, SEM, XRD, EDAX, TGA, and AFM.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Qing Li,Yong You,Xingyu Hu,Danqing Lu,Qian Wen,Gang Yu,Wenlei Wang,Tao Xu
This work innovatively used cellulose nanofibers as a photocatalyst carrier, which could recycle nano-photocatalysts and minimize nanoparticle aggregation. The morphology, structures, chemical composition, optical-electronic properties and photocatalytic performance of amino-modified carbon quantum dots-ZnO/cellulose nanofiber (N-CQDs-ZnO/CNF: ZCH-2) hydrogel were characterized by SEM, TEM, BET, EDS , XRD, FTIR, UV–vis, XPS, PL and other techniques. The mechanism of Cr(VI) adsorption synergistic photoreduction by ZCH-2 was discussed in detail. The results showed that the prepared ZCH-2 had excellent removal performance for Cr(VI). After 120 min of adsorption and 40 min of photoreduction, the removal efficiency of Cr(VI) was 98.9 %. Compared with ZnO/CNF hydrogel, the adsorption performance of ZCH-2 increased by 268 % and the photoreduction performance increased by 116 %. The adsorption of Cr(VI) by ZCH-2 was controlled by electrostatic attraction and chemical adsorption. The photoreduction kinetic constant of ZCH-2 was 0.106 min −1 , which was 8.9 times that of ZnO/CNF hydrogel. The N-CQDs in ZCH-2 could form N-CQDs-metal complexes with Cr(VI), resulting in fluorescence quenching , so Cr(VI) could be visually identified by fluorescence changes. This study provides a new idea for the design and optimization of a new multifunctional hydrogel with efficient adsorption-photoreduction-fluorescence recognition.
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高影响因子
ACS ES&T Engineering
·
2023
·
IF 7.1
Huan Tang,Shimao Deng,Zheting Chu,Yangzi Shangguan,Jiaxin Liang,Qian Zheng,Ranhao Wang,Hong Chen
Simultaneously reducing and immobilizing Cr(VI) anions in groundwater are crucial to minimize their hazardous effects. Herein, benefiting from the feasible chemical-/photo-reduction capability of greigite, together with the ion-exchange functionality of zeolites, the integrated three-in-one function in greigite/Re-ANA composites (GRAs) material has been employed for removing and immobilizing Cr(VI) in groundwater remediation. GRA-3 achieved a 99.4% Cr(VI) removal efficiency in a Cr(VI) solution with 1 mg/L. Cr(VI) residue concentration is 0.006 mg/L, complying with the control guideline in drinking water according to WHO regulations. A comprehensive mechanism study reveals that the chemical reduction and photoreduction processes are involved within greigite, which drives the process of reducing Cr(VI) to Cr(III). Subsequently, the as-reduced Cr(III) is either adsorbed on a greigite surface or ion-exchanged with zeolite microporous channels, thus getting immobilized. Furthermore, environmentally relevant Cr(VI) contaminated groundwater sampling from the chromate plant has been employed for the fixed-bed column study, which achieved the discharge standard for practical Cr(VI) polluted groundwater. This work reported a composite material matrix with great potential and significance for Cr(VI) remediation, which could be employed in permeable reactive barriers for Cr(VI)-polluted groundwater remediation in the future.
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LANGMUIR
·
2023
·
IF 3.9
Wenjing Zhu,Zhinan Xia,Bingfeng Shi,Changli Lü
A series of 2D M(Cu, Zn, Co, and Mn)-TCPP MOFs/TiO2 binary nanocomposites (TCPP = tetrakis(4-carboxyphenyl)porphyrin) were constructed by solvothermal in situ loading of flaky TiO2 on the surface of 2D metal–organic frameworks (MOFs). The influence of different coordination metals on the catalytic activity was studied, and it was found that the 2D Cu-TCPP MOFs/TiO2 nanocomposite exhibited the best photo-Fenton performance. The superior property can be attributed to the high absorption coefficient and ultrathin two-dimensional structure of the 2D Cu-TCPP MOFs nanosheets. Meanwhile, the 2D Cu-TCPP MOFs/TiO2 II heterostructure can effectively promote the separation and transfer of photoformed carriers. Moreover, under visible irradiation, the optimized 2D Cu-TCPP MOFs/TiO2 composite can convert 99.9% of Cr(VI) to Cr(III) within 60 min with methanol as the hole scavenger at pH 3.14. Also, the photocatalytic performance of 2D Cu-TCPP MOFs/TiO2 was maintained after five reaction cycles. Furthermore, the proposed visible-light-driven photocatalysis mechanism of the 2D Cu-MOFs/TiO2 composite was reasonably derived according to experimental results. This study demonstrates the potential of building efficient TiO2-based visible light photocatalysts with 2D metal-porphyrin MOFs.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 22
·13306-13319
·
IF 12.732
Qian Yang,Huilin Wang,Fangbai Li,Zhi Dang,Lijuan Zhang
Chromium is recognized as one of the most harmful heavy metal pollutants. Facile and efficient Cr(VI) removal technology is an urgent need, but still a challenge. Here, a novel core–shell magnetic mesoporous polydopamine nanocomposite adsorbent (Fe3O4@mesoPDA) was prepared by in situ polymerization of dopamine on the surface of Fe3O4 nanoparticles. The adsorption of Cr(VI) was highly pH-dependent, and optimal Cr(VI) adsorption occurred at pH = 1.5 with a maximum adsorption capacity of 574.71 mg g−1. The adsorption kinetics results showed that the large-sized mesoporous polydopamine shell layers of Fe3O4@mesoPDA significantly increased the adsorption sites and removal rate of Cr(VI), and its inner core Fe3O4 nanoparticles could also accelerate Cr(VI) removal. The adsorption mechanisms of Fe3O4@mesoPDA were primarily redox reactions and also involved electrostatic interactions and coordination. Cr(VI) was mainly reduced to Cr(III) by catechol and imino groups of PDA shell layers, but the pathway of the superoxide radical reduction of Cr(VI) mediated by iron ions on the surface of Fe3O4 nanoparticles could promote the electron transfer between PDA shell layers and Cr(VI) and greatly improve the adsorption performance of Fe3O4@mesoPDA, especially under weak acid conditions. Meanwhile, newly generated Cr(III) was further immobilized onto Fe3O4@mesoPDA through coordination with N and O functional groups and recovered by magnetic separation in favor of decreasing the environmental hazard of heavy metal Cr. Overall, this work can provide new insights into the interaction mechanisms between PDA-based adsorbents and Cr(VI), and also offers a significant reference for the subsequent preparation of Cr(VI) adsorbents.
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