Water
·
2025
·Vol. 17
·期 19
·2910
·
IF 3
Xinchi Zong,Tianliang Duan,Linyan Chen,Zhengwei Luo,Hui Jiang,Wenhua Geng
The escalating issue of water pollution driven by rapid industrialization necessitates the development of advanced remediation technologies. In this study, a novel method for producing chromium (Cr(VI)) ion-imprinted biochar (Cr(VI)-IIP-PEI@NBC) from wheat residue was proposed. After acid-oxidative modifications, polyethyleneimine (PEI) and glutaraldehyde (GA) were employed as the functional monomer and crosslinker, respectively, to enhance the biochar’s selectivity and adsorption capacity. Under optimized conditions (pH 2.0, 55 °C), the adsorbent achieved a maximum Cr(VI) uptake of 212.63 mg/g, which was 2.3 times higher than that of the non-imprinted biochar. The material exhibited exceptional specificity (99.64%) for Cr(VI) and maintained >80% adsorption efficiency after five regeneration cycles, demonstrating excellent reusability. Comprehensive structural characterization via Fourier transform infrared spectroscopy (FT-IR), thermal gravimetric analysis (TGA), Brunner–Emmet–Teller measurements (BET), and Scanning Electron Microscopy (SEM) confirmed successful Cr(VI) imprinting in the biochar and its high thermal stability and mesoporous architecture, elucidating the mechanisms behind its superior performance. This study presents a sustainable and high-performance adsorbent for the efficient treatment of chromium-contaminated wastewater, with significant potential for industrial applications.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Linshan Zhang,Guozong Yue,Luming Yang,Deshun Huang
Ultra-thin MXene nanosheets (Nss) were facilely prepared via delaminating and intercalating the multi-layered MXene using tetramethylammonium hydroxide (TMAOH). Electron-rich characteristics, abundant surface active sites and the negative charges made MXene Nss having both good reduction ability and adsorption capacities, which would effectively remove anion Cr(VI) via reduction and remove cation Cr(III) via adsorption. Batch adsorption tests were carried out to study the pH impact, adsorption kinetics and isotherms. Upon adsorption, the well dispersed MXene Nss suspension was aggregated to form flocs and sediment at the bottom. The maximum Cr(VI) and Cr(III) removing capacities are calculated to be 554.9 mg/g at 318 K and 283 mg/g at 298 K, respectively. The mechanisms on Cr(VI)/Cr(III) adsorption were well studied employing SEM, TEM , XPS and FT-IR. In addition, the MXene Nss also showed good adsorption capacity towards other metal cations (such as Cu 2+ , Cd 2+ , and Pb 2+ ), manifesting that the current MXene Nss has the potential to be used as a general-purpose adsorbent.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chen Wang,Mingjie Huang,Wentao Hu,Wei Xiang,Tao Zhou,Juan Mao,Feixiang Zan,Xiaohui Wu
The carcinogenic and hard-to-dispose Cr(VI) in high-salinity industrial wastewater has caused severe environmental problems. Herein, a novel hollow spherical CuFe 2 O 4 spinel oxide with concentrated confined oxygen vacancies (HS/CuFe 2 O 4 -OVs) was developed for Cr(VI) decontamination. Such a fancy material delivers a remarkable removal rate of 0.041 min −1 , approximately-one order of magnitude higher than the commonly reported iron-based materials. The OVs in the confined space could exert dual effects on Cr(VI) removal from the aspects of enhanced stabilization via local electronic structure regulation and strengthened immobilization via electron conductivity modulation. Importantly, due to the highly sensitive response of Cr(VI) to the changed confined OVs content, the HS/CuFe 2 O 4 -OVs showed higher selectivity for Cr(VI) removal in the interference of high concentration salts than its nonhollow-structured counterpart and can successfully treat Cr(VI)-contaminated industrial wastewater with high salinity. This work opens up a new concept for rational design of robust spatial confined architectures for Cr(VI) treatment.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Boyu Jia,Tianbao Liu,Juanjuan Wan,Andrei Ivanets,Yujia Xiang,Lijuan Zhang,Xintai Su
Microbial reduction of hexavalent chromium (Cr (VI)) shows better efficiency and cost-effectiveness. However, immobilization of Cr (III) remains a challenge as there is a limited supply of electron donors. A greener and cleaner option for donating external electrons was using bioelectrochemical systems to perform the microbial reduction of Cr(VI). In this system, we constructed a polydopamine (PDA) decorated Shewanella oneidensis MR-1 ( S. oneidensis MR-1) bioelectrode with bidirectional electron transport, abbreviated as PDA@ S. oneidensis MR-1. The conjugated PDA distributed on the intracellular and extracellular of individual S. oneidensis MR-1 has been shown to accelerate electron transfer by outer membrane C-type cytochromes and flavin-bound MtrC/OmcA pathway by various electrochemical analyses. As expected, the PDA@ S. oneidensis MR-1 biofilm achieved 88.1% Cr (VI) removal efficiency (RE) and 58.1% Cr (III) immobilization efficiency (IE) within 24 h under the autotrophic conditions at the optimal voltage (−150 mV) compared with the control potential (0 mV). The PDA@ S. oneidensis MR-1 biofilm showed increased RE activity was attributed to the shortening of the distance between individual bacteria by PDA. This research provides a viable strategy for in situ bioremediation of Cr(VI) polluted aquatic environment.
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Polymer-Plastics Technology and Materials
·
2023
·
IF 2.7
Qianyong Liang,Ying Pan,Jia Du,Dong Zhang,Yan Zhang,Zhishun Zhong,Hongting Zhao
Carbon sphere@layered double hydroxides filled cellulose nanofibers (ACS@LDHs/CNF) aerogel was successfully synthesized. The removal rate of Cr(VI) using ACS@LDHs/CNFs aerogel at a solid-liquid ratio of 1 g/L was 89.4%, which was higher compared to the removal rate of 65.2% using LDHs alone. The adsorption capacity of ACS@LDHs/CNFs for Cr(VI) was determined to be 44.9 mg/g. The adsorption kinetics followed the pseudo-second-order kinetic equation, and the isotherm data showed good agreement with the Langmuir model. The adsorption mechanism of Cr(VI) onto ACS@LDHs/CNFs aerogel was also investigated. Additionally, the ACS@LDHs/CNFs aerogel demonstrated consistent high adsorption efficiency over 4 consecutive cycles of adsorption-regeneration.
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CHEMOSPHERE
·
2023
·
IF 8.8
Aikui Chen,Yao Huang,Hui Liu
Sulfidated nanoscale zerovalent iron (S-nZVI) has been extensively studied for the reductive removal of Cr(VI), but its applicability is limited by agglomeration and unexpected efficiency reduction. In this study, chitin microsphere supported sulfidated nanoscale zero-valent iron (S-nZVI@Chi-M) was prepared by in-situ one-step reduction method and used to remove Cr(VI) from water. Compared to chitin and chitosan powder, Chi-M with nanofibrous structure and large surface area performed best in stabilizing S-nZVI with a Fe 0 loading content of 3.01 wt%. The S-nZVI particles were homogeneously distributed on the surface of Chi-M, effectively avoiding agglomeration. Compared with bare nanoparticles and supported nZVI, S-nZVI@Chi-M showed significantly enhanced Cr(VI) removal capacity (924.5 mg Cr(VI) for per gram of effective Fe 0 ). The influences of sulfidation degree, dosages, initial Cr(VI) concentration, pH, DO, humic acid and typical ions on Cr(VI) removal kinetics were further studied. S-nZVI@Chi-M could be recycled for at least 4 times with acceptable reactivity. The mechanism investigation results indicated that the Cr(VI) removal was a complex process of reduction, adsorption and co-precipitation under the synergistic effect of Chi-M and S-nZVI. This work provides new ideas for the continuous fabrication of highly reactive nanoparticles, hopefully expanding the application scope of biomass resources in pollution remediation.
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Polymers
·
2023
·Vol. 15
·期 13
·2918
·
IF 5
Cheng Tang,Tao Hu,Chengzhen Du,Ziqin Liao,Wenyan Cheng,Fen Wang,Xiaoli Hu,Kunpeng Song
A Fe-N conjugated organic polymer (SMP-Fr-Py) was prepared from ferrocene and pyrrole using a Scholl coupling reaction, which significantly improved the performance of Cr(VI) removal compared to the polymer (HCP-Fr-Py) prepared by adding the cross-linker formaldehyde dimethyl acetal (FDA). The results showed that at a pH of 2 and at 25 °C, the removal of Cr(VI) reached 90% for SMP-Fr-Py and only 58% for HCP-Fr-Py after 20 min of reaction. Subsequently, 99% and 78% were achieved after 120 min of reaction, respectively. The test results showed that the removal reaction followed a pseudo-second-order kinetic model. The removal efficiency decreased with increasing solution pH and initial Cr(VI) concentration, but increased with increasing SMP-Fr-Py dosage, reaching three cycles. The characterization of the reaction complexes and measurements of Cr species conversion revealed the near absence of Cr(VI) species in the solution. Approximately 38% of Cr(VI) was found to be adsorbed on the material surface, with another fraction present in solution (24%) and on the material surface (38%) in the form of Cr(III). The overall study showed that the direct connection of ferrocene and pyrrole in SMP-Fr-Py through C-C bonding increased the conjugated structure of the polymer backbone, which facilitated electron transfer and transport. Furthermore, the Fe-N elements worked synergistically with each other more easily, which improved the removal performance of Cr(VI) and provided a reference for the subsequent work.Keywords:organic polymers;Fe-N co-doping;Cr(VI) removal;conjugate structure
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tong Zhang,Yuan Chen,Yurong Zhang,Bin Liu,Yuanyuan Liu,Jianwei Zhao
Cr(VI) and catechol are common pollutants in wastewaters of tannery industry. Cr(VI) reduction by catechol results in accumulation of Cr(V)-complex and toxic o -benzoquinone. Cr(VI) reduction can be enhanced by accelerating the electron transfer from catechol to Cr(VI) using Fe(III). This electron transfer allows the continuous production of reactive oxygen species (ROS) in advanced oxidation processes, which further degrades catechol. However, the effects of catechol on Fe(III)-based Cr(VI) reduction and ROS production are not clear. In this study, the electron transfer pathway between catechol, Fe(III) and Cr(VI) was investigated along with the catechol degradation by ROS. Results show that the process of Cr(VI) reduction follows well a pseudo-second-order kinetic model, and the activation energy decreases by 4189 J/mol after electrons are transferred by Fe(III). Aqueous chromium (50 mg/L) was completely precipitated as Cr(OH) 3 , Fe x Cr 1-x (OH) 3 or Fe(OH) 3 -Cr(OH) 3 at Fe(III) concentration of 10 mmol/L. Residual catechol and Fe(II) in wastewater activated percarbonate, thereby producing OH for over 480 min at pH 3.0 and generating OH and CO 3 − for over 5 min at pH 10.0. Catechol was degraded by these ROS to butenedioic, oxalic, and formic acids, which were then mineralized to H 2 O and CO 2 . Catechol (2 mmo/L) was fully removed from wastewater with TOC removal of 37%, and the degradation was not affected by SO 4 2− and Cl − . This study provides new insights into the removal of pollutants from wastewaters via electron transfer mediated by Fe(III), and may aid in controlling the toxic effects of Cr(VI) and catechol-like organics in natural and engineered aquatic systems.
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Separations
·
2023
·Vol. 10
·期 6
·358
·
IF 2.6
Xiangfen Cui,Juan Wang,Qun Zhao,Chen Li,Jianhong Huang,Xuewei Hu,Jie Li,Mantao Li
Biochar adsorption has emerged as a favorable and environmentally friendly approach for removing metals such as chromium (Cr) from wastewater. However, the use of pristine biochar (PBC) is limited due to its finite adsorptive capacity, selectivity, and potential for secondary pollution. In this study, a novel bifunctionalized magnetic biochar (BMBC) was fabricated by incorporating cystamine as a ligand and glutaraldehyde as a crosslinker into alkali-treated magnetic biochar (MBC). This chemical modification introduced numerous amino groups and disulfide bonds onto the surfaces of BMBC. The biochar adsorbents’ surface morphologies, crystal structures, and texture properties were characterized using SEM, XRD, and N2adsorption-desorption techniques. The specific surface area was determined using the BET method. Furthermore, the surface functional groups and elemental compositions before and after adsorption were analyzed using FTIR and XPS, respectively. The results demonstrated higher Cr(VI) removal efficacy of BMBC (100%) than MBC (72.37%) and PBC (61.42%). Optimal conditions for Cr(VI) removal were observed at a solution pH of 2, a temperature of 50 °C, a reaction time of around 1440 min, and an initial adsorbate concentration of 300 mg/L. The sorption process followed a chemical mechanism and was controlled by monolayer adsorption, with a maximum adsorption capacity of 66.10 mg/g at 50 °C and a pH of 2, as indicated by the larger fitting values of the pseudo–second-order and Langmuir models. The positive ∆Hoand ∆Sovalues and negative ∆G0 values suggested a spontaneous and endothermic Cr(VI) adsorption process with high randomness at the solid/liquid interface. The removal of Cr(VI) was attributed to the reduction of Cr(VI) into Cr(III) facilitated by the introduced amino acids, sulfur, and Fe(II), electrostatic interaction between Cr(VI) in the solution and positive charges on the adsorbent surface, and complexation with functional groups. The presence of co-existing cations such as Cu(II), Cd(II), Mn(II), and K(I) had little effect on Cr(VI) removal efficiency. At the same time, the co-existence of anions of Cl−, NO3−, SO42−, and HPO42−resulted in a 7.58% decrease in the Cr(VI) removal rate. After five consecutive adsorption/desorption cycles, BMBC maintained a high Cr(VI) removal rate of 61.12%. Overall, this novel BMBC derived from rice straw shows great promise as a biosorbent for treating Cr(VI) in wastewater.Keywords:magnetic biochar;bifunctionalization;chemical modification;hexavalent chromium;adsorption
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Cheng Yu,Xiaoxi Zhu,Abdelkader Mohamed,Ke Dai,Peng Cai,Shilin Liu,Qiaoyun Huang,Baoshan Xing
Biochar can act as a shuttle to accelerate the extracellular electron transfer (EET) by exoelectrogens. However, it is poorly understood how the persistent free radicals (PFRs) in biochar affected EET and the redox reaction. Herein, the effects of the biochar and chitosan modified biochar (CBC) on the Cr(VI) bioreduction by Shewanella oneidensis MR-1 (MR-1) was investigated. Kinetic study indicated that the Cr(VI) bioreduction rate constant by MR-1 was increased by 1.8–33.7 folds in the presence of biochar, and by 2.7–60.2 folds in the presence of CBC, respectively. Moreover, Cr(VI) bioreduction rates increased with the decreasing pH. Results suggested that the electrostatic attraction between Cr(VI) and redox-active particles could accelerate the EET by c -cytochrome due to the promotion of the Cr(VI) migration from aqueous phase to biochar or CBC. Electron paramagnetic resonance analysis suggested that the PFRs affected the electron transfer from the ·O 2 - generated by MR-1 to Cr(VI) and accelerate the Cr(VI) bioreduction. Remarkably, in the presence of PFRs, this electron shuttling process was dependent on the non-metal-reducing respiratory pathway. Our results offer new insights that free radicals may be widely involved in the EET and strongly impact on the redox reaction in the environment.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Tao Xian,Hongqin Li,Xiaofeng Sun,Yashan Huo,Lijing Di,Chenyang Sun,Hua Yang
The In2O3 nanoparticles were homogeneously attached on the BiOBr nanoplate surface to obtain S-scheme In2O3/BiOBr heterojunction photocatalysts by a hydrothermal route. The purity, crystal structure, chemical state, morphology, light absorption property, and photogenerated charge behavior of composites were investigated by XRD, SEM, TEM, HRTEM, XPS, UV–vis DRS, PL, ESR, and electrochemical tests. The removal of dyes (acid orange 7 (AO7), acid orange 10 (AO10), and rhodamine B (RhB)) and Cr(VI) was employed to evaluate the photocatalytic performance of In2O3/BiOBr composites irradiated by simulated sunlight. The results indicate that the photocatalytic performance of BiOBr can be remarkably promoted after the decoration of In2O3 nanoparticles, and the best photocatalytic activity was achieved over an 8% In2O3/BiOBr sample. The 8% In2O3/BiOBr sample also indicates outstanding synergistic photocatalytic performance for the removal of the heavy metal ion/dye mixture (AO7/Cr(VI) and RhB/Cr(VI)). It is found that the decoration of In2O3 nanoparticles can accelerate the transfer and separation of photoinduced electrons and holes in BiOBr nanoplates. The energy band structure, work function, and Fermi level of BiOBr and In2O3 were computed through the density functional theory calculation. Based on the above investigation, the photocatalytic mechanism of the S-scheme In2O3/BiOBr composite was discussed.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Yunquan Liu,Huimei Shan,Yanyue Pang,Hongbin Zhan,Chunya Zeng
Iron modified chitosan/coconut shell activated carbon (Fe/CSCC) composite bead is synthesized to remove Cr(VI) and is characterized to reveal the influencing factors and reaction mechanism. Results show that the adsorption capacity ( Q e ) of Cr(VI) increases with the increase of iron loading, contact time ( t ), Cr(VI) initial concentration ( C 0 ), and temperature ( T ), but decreases with the increase of pH, and mass and volume ratio ( m/v ). After 0.1 mol FeCl 3 modification, the removal efficiency of Cr(VI) by Fe/CSCC reaches as high as 97.25 % at pH = 3, m/v = 1.0 g/L, t = 2880 min, C 0 = 25 mg/L, and T = 25 °C. The coexisting ions of SO 4 2− , HPO 4 − , and Ca 2+ lead to the decrease of Q e by 7.82, 5.05, and 5.50 mg/g, respectively, and the inhibition effect increases with their increasing concentrations. Fe/CSCC adsorption for Cr(VI) is an endothermic spontaneous process, and a chemical and monolayer adsorption, which is better fitted to a pseudo-second-order kinetic. The fitted maximum Q e is 64.49 mg/g by using the Langmuir model. Moreover, after five cycles of regeneration, the Q e value only drops about 3.46 mg/g. Characterization analysis of BET, XRD , FTIR , XPS, and SEM-EDS indicates that Cr(VI) is mainly adsorbed by Fe/CSCC through electrostatic attraction and complexation, which is related to the −COOH and − NH 2 groups, and Fe − O groups, respectively.
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