TALANTA
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2024
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IF 5.6
Cheng Yao,Yi Cai,Yali Gong,Yong Zhao,Qing Chen
Microplasma jet (MPJ), serving as excitation sources in miniaturized systems, has been widely used for contaminant detection. However, the employment of the MPJ is conditioned due to the limit generation of the radicals. Here, a novel 4-channel microplasma jet array (MPJA) is designed for 3,3,5,5-tetramethylbenzidine (TMB) rapid oxidation without oxidizing reagents and catalysts. The jet array, generated from a ceramic tube, allows direct contact with the sample. A colorimetric system containing the MPJA has been developed for the detection of hexavalent chromium. Compared to the MPJ, the employment of MPJA significantly makes the detection system effective and sensitive. Under optimal operating condition, the system exhibits a linear response for Cr (VI) detection within the range of 0.3–1.2 μmol L −1 , with a detection limit (LOD) of 0.11 μmol L −1 . The practicality of the system is validated through the analysis of real-world samples. The system can be packed into a case with 40 cm in length, 30 cm in width and 30 cm in height. The power consumption is 0.052 W. The system provides a potential method for samples determination in emergency.
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CHINESE CHEMICAL LETTERS
·
2024
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IF 9.4
Yan-Kai Zhang,Yong-Zheng Zhang,Chun-Xiao Jia,Fang Wang,Xiuling Zhang,Yuhang Wu,Zhongmin Liu,Hui Hu,Da-Shuai Zhang,Longlong Geng,Jing Xu,Hongliang Huang
ABSTRACT The highly desired goal is to employ visible light for the photocatalytic reduction of toxic Cr(VI) to environmentally friendly Cr(III). Metal-organic frameworks (MOFs) are considered one of the most promising materials for the photoreduction of Cr(VI). Nevertheless, developing MOFs with high stability and activity is still challenging. Herein, we report a stable Zn-based MOF (named DZU-64 ) with an anthracene functionalized ligand, and its reduction of Cr(VI) under sunlight irradiation was investigated. DZU-64 exhibits excellent chemical stability in pH range of 2−14 aqueous solution, and remarkable thermal stability to 570°C. For the photoreduction of Cr(VI) under visible light irradiation, DZU-64 gives a record rate constant of 0.467 min −1 and a high Cr(VI) reduction rate of 6.68 mg Cr (VI) g −1 cata min −1 at pH 2. Moreover, under real solar light, DZU-64 can also efficiently reduce Cr(VI) to Cr(III) while retaining its catalytic activity throughout 5 cycles without any notable decline, further demonstrating its great application prospect. By combining the photovoltaic performance tests and electron spin resonance test, the possible photoreduction of Cr(VI) mechanism in DZU-64 was analyzed.
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LANGMUIR
·
2024
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IF 3.7
Chun Hu,Yaodong Xiao,Qingrong Jiang,Mengyao Wang,Tingdan Xue,Ruidong Tao,Yunjun Mei
Microplastics (MPs) are novel pollutants that can adsorb heavy metals in water environments and migrate together as carriers and are prone to aging due to the light in water. However, few reports have been published on the synergistic behavior and effects of these different types of aged MPs on the adsorption and desorption of Cr(VI). Here, two MP types─polyamide (PA) and polylactic acid (PLA)─were aged by UV irradiation, and the adsorption and desorption behaviors of MPs on Cr(VI) were studied. The results indicated that UV light can rapidly age MPs. After the MPs were exposed to UV light, their specific surface area, negative charge, and oxygenic groups increased, resulting in enhanced hydrophilicity. The aged MPs depicted a markedly enhanced adsorption capacity for Cr(VI) compared with the results of aged-PA > pristine-PA > aged-PLA > pristine-PLA. The process followed the Langmuir and pseudo-second-order models, confirming that chemical and monolayer adsorption are the primary processes involved in the adsorption of Cr(VI) by aged MPs. Cr(VI) was more easily desorbed in the simulated gastric fluid environment. The desorption rate of aged MPs was lower than that of pristine MPs because of their stronger binding forces to Cr(VI). The binding of Cr(VI) to MPs mainly depends on synergistic mechanisms such as electrostatic attraction, reduction reactions, and chelation of oxygenic groups. This study clarifies the reciprocity mechanism between aging MPs and Cr(VI) and provides further insights and guidance for controlling the joint pollution between MPs and heavy metal pollutants in the future.
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Environmental Science & Technology Letters
·
2017
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IF 5.308
Jun-Cheng Han,Guo-Jun Chen,Li-Ping Qin,Yang Mu
Cr isotope fractionation during microbial reduction processes is commonly recognized as a promising tool in biogeochemistry and bioremediation. However, the mechanism of Cr isotope fractionation during microbial reduction is poorly understood. In this work, the relationship between the bacterial respiratory pathway and Cr isotope fractionation was investigated in Shewanella oneidensis MR-1. For comparison with the wild type, a mutant strain (ΔomcA/ΔmtrC) with a deficiency in extracellular Cr(VI) reduction was constructed by deleting the omcA and mtrC genes, which encode the terminal reductase during extracellular reduction. The magnitudes of Cr isotope fractionation (ε) for Cr(VI) reduction by the wild type and ΔomcA/ΔmtrC were −2.42 ± 0.68‰ and −2.70 ± 0.22‰, respectively. Surprisingly, the ε values were not significantly different between the two strains. This suggests that isotope fractionation is independent of the metal respiratory pathway during Cr(VI) reduction by S. oneidensis MR-1. Moreover, a three-step Cr isotope fractionation model that includes uptake, reduction, and efflux was proposed to exist during intracellular Cr(VI) reduction by S. oneidensis MR-1. The developed model provides a better understanding of Cr isotope fractionation during microbial reduction.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Lin Yang,Zhou Yuan,Lufang He,Le Han,Bohan Li,Yan Xu
The design and intentional construction of crystalline materials containing two clusters with redox properties in one framework still remains challenging. Linking oxidative polyoxometalate (POM) clusters and a reductive cyclic trinuclear copper complex (Cu-CTC) to prepare stable catalysts is rarely reported. Herein, we successfully obtained two new polyoxometalate-based metal–organic compounds (POMOCs) [CuII3(PyCA)3(μ3-OH)(β-Mo8O26)0.5(H2O)2]·5H2O (1), [CuII3(PyCA)3(μ3-OH)]2(CuIIW12O40)[CuII(H2O)6] (2) (PyCA = 1H-pyrazole-4-carbaldehyde) by enabling precursors of Cu-CTC and POM cocrystallization in one pot via hydrothermal method. The [β-Mo8O26]4– cluster in compound 1 combined with Cu-CTC units to form a 1D structure, and the [CuW12O40]6– unit in compound 2 linked two Cu-CTC units to form a sandwich-like 0D structure. Also, Cu-CTC CuI3(PyCA)3·H2O (Cu3) was synthesized for performance comparison. A series of characterizations indicate that compound 1 is more conducive to electron transfer than compound 2. In addition, compounds 1 and 2 can act as bifunctional catalysts for the electrochemical detection and photocatalytic reduction of Cr(VI). Particularly, the photoreduction rates of Cr(VI) by compounds 1 and 2 are 96.7% and 96.3% for only 10 and 14 min under visible light, respectively, and it is better than that of Cu3 and most other reported photocatalysts. Furthermore, the active sites and mechanisms for electrochemical detection and photocatalytic reduction of Cr(VI) were discussed.
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JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Tongxin Xiao,Kangyue Qiao,Guodong Hao,Songyao Du,Yue Wang,Chao Sui
This study employed a solvothermal method to prepare an NH 2 -MIL-101(Fe, Co) bimetallic organic framework composite catalyst aimed at enhancing the photocatalytic reduction performance of Cr(VI). The experimental results show that introducing Co into the single-metal NH 2 -MIL-101(Fe) does not alter the material's octahedral structure. However, the bimetallic synergistic effect shifts the light absorption range to the red end of the spectrum, reduces the bandgap, and significantly improves carrier separation efficiency. Under visible light irradiation, the NH 2 -MIL-101(Fe, 0.15Co) catalyst exhibited outstanding photocatalytic performance, achieving a reduction efficiency of 94.7% for Cr(VI) within 40 minutes and 100% within 50 minutes, with a reaction rate constant 4.7 times that of the single-metal NH 2 -MIL-101(Fe). Free radical capture experiments further revealed that ·O 2 - is the key active species in the Cr(VI) reduction process, while photo-generated holes in the valence band can oxidise OH - to ·OH, synergistically participating in the reaction. Additionally, cyclic stability experiments showed that the catalyst maintained 85.8% reduction efficiency after five cycles, demonstrating excellent stability and practical application potential.
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ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Li Song,Weiguo Zhang,Quan Liu,Xiao Zhang,Fuqiang Liu,Aimin Li
Various organic acids commonly coexist with Cr(VI) in wastewater. However, direct electron transfer between Cr(VI) and electron-rich organic acids is typically slow. Current Fe-based mediators primarily operate through the aqueous Fe(III)/Fe(II) cycle, which faces challenges in achieving efficient Fe recycling. To address the efficient removal of Cr(VI) and sodium citrate (Cit) composite pollutants (Cr(VI)-Cit), iron-loaded carbon nitride composites (Fe/CN) were synthesized via a combined loading-calcination approach. Crucially, coordination between carboxylate groups of Cit and undercoordinated Fe sites on Fe/CN formed photoactive complexes, effectively stimulating ligand-to-metal charge transfer (LMCT). This significantly enhanced the solid-phase Fe(III)/Fe(II) cycling efficiency, leading to a markedly increased Cr(VI) reduction rate constant ( k ) of 0.213 mg/(L·min). Furthermore, coordination with the N-rich matrix effectively inhibited Fe leaching, resulting in a post-reaction total Fe concentration below 0.5 mg/L. The formation of a Cr(VI)-Fe-Cit ternary cyclic complex effectively lowered the activation energy for Cr(VI) reduction by 81.3% compared to pristine CN. In the dark, intramolecular electron transfer within this complex generated Fe(II)-Cit species with a low electrode potential. Under irradiation, the photoactive Fe(III)-Cit complex generated Fe(II) via LMCT to reduce Cr(VI); concurrently, photogenerated electrons (e - ) and superoxide radicals (·O 2 - ) also contributed to Cr(VI) reduction. Reusability tests showed Fe/CN retained ∼90% Cr(VI) removal efficiency from actual wastewater over 5 cycles, demonstrating good stability under realistic conditions. This study provides valuable insights for the cost-effective and efficient remediation of Cr(VI)-organic acid complexes in real wastewater.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Huirong Zhang,Yi Shen,Jinglei Cui,Baofeng Wang,Yanxia Guo,Dongke Zhang,Fangqin Cheng
s Lignin-derived carbonaceous materials have emerged as promising candidates for heavy metal remediation owing to their low cost, tunable surface chemistry, and hierarchical porosity. In this study, a FeCl 3 –urea co-activation strategy was employed to synthesize N-doped hierarchical porous carbons (N-HPCs) from lignin for efficient Cr (VI) removal. The synthesis parameters were systematically optimized using a machine learning (ML) workflow, with experimental data serving as the training set. Gradient boosting regression (GBR) achieved high predictive accuracy (R 2 = 0.86), and SHAP-based feature importance analysis identified pyridinic-N (N-5) content as the dominant factor governing Cr (VI) adsorption, attributed to its redox-active nature. Under optimal conditions (FeCl 3 :lignin:urea = 3:1:0.5), the resulting N-HPC exhibited a high specific surface area (2297.5 m 2 /g), elevated N-5 content (67.08%), and a maximum Cr (VI) adsorption capacity of 627.1 mg/g. Mechanistic studies revealed that reduction–complexation, primarily facilitated by N-5 sites, accounted for up to 87.7% of Cr (VI) removal. The ML-driven inverse design strategy further predicted that precise control of N-5 levels could yield N-HPCs with adsorption capacities exceeding 650 mg/g. This work demonstrates the synergy of ML-guided optimization and mechanistic insight, providing a robust framework for the rational design and accelerated development of sustainable, high-performance adsorbents for heavy metal remediation.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
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IF 5.4
Yongshan Ma,Qingxiang Guan,Huayun Zang,Fengxia Zhang,Tianyi Jiang,Xuemei Li,Yanyan Zhu
Solar-driven photocatalysis is a promising green technology for wastewater treatment. Molybdenum disulfide (MoS 2 ) is a highly efficient visible-light photocatalyst. However, due to the rapid recombination of photoinduced electron-hole (e - -h + ) pairs, its photocatalytic activity is severely limited, thereby hindering its practical application. To solve this problem, a novel MoS 2 -3,4,9,10-perylene tetracarboxylic acid (MoS 2 -PTCDG) heterojunction was synthesized via a hydrothermal method. In this composite, PTCDG nanosheets are embedded in the interlayer spaces of three-dimensional flower-like MoS 2 nanospheres, forming an organic–inorganic heterostructure. This design not only improves the separation efficiency of photogenerated e - -h + pairs, but also the hydrophilic terminal carboxyl groups on PTCDG can serve as adsorption sites for Cr(VI) pollutants. The MoS 2 -PTCDG composite demonstrates exceptional photocatalytic activity and stability in degrading Cr(VI) under simulated sunlight, achieving a reaction rate constant 2.5 times higher than that of pure MoS 2 . This study highlights the potential of rationally designed organic–inorganic heterostructures to overcome the limitations of traditional MoS 2 -based photocatalysts, thus offering new insights into the development of high-performance photocatalytic materials for environmental remediation.
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Surfaces and Interfaces
·
2025
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IF 6.3
Tang Xiaojing,Shakeel Zeb,Hao Li,Abdul Haleem,Zhong Hua
The removal of hexavalent chromium from wastewater is a pressing environmental challenge due to its high toxicity and strong mobility in aquatic systems. To address this issue, we engineered a three-dimensional porous biomonolith via redox cryopolymerization, leveraging the abundant functional groups and structural advantages of covalently crosslinked lignin and chitosan for efficient chromium adsorption. Remarkably, the developed biomonolith exhibited a high chromium adsorption capacity of 232.2 mg/g at pH 2, reaching 63.6% of equilibrium uptake within the first 30 min and achieving full equilibrium in 90 min. This enhanced performance stems from the synergistic effects of the material’s macroporous structure, which facilitates rapid chromium diffusion, and its multifunctional surface chemistry, featuring amine, amide, sulfonic, and oxygen-containing groups. These functional groups promote chromium adsorption through electrostatic interactions and partial reduction of Cr(VI) to Cr(III), as confirmed by X-ray photoelectron spectroscopy (XPS). The positively charged Cr(III) further strengthens electrostatic interactions with lignin’s oxygen-containing groups, enhancing adsorption. The chromium adsorption process followed the pseudo-second-order kinetic model (R² = 0.972) and the Freundlich isotherm (R² = 0.93), indicating chemisorption and surface complexation as the dominant mechanisms. The developed biomonolith exhibits enhanced selectivity, improved shelf stability, and excellent reusability for chromium adsorption. This lignin-based biomonolith presents a promising solution for Cr(VI) removal, offering significant potential for environmental applications and advancing research in sustainable wastewater treatment.
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ACS Applied Materials & Interfaces
·
2018
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IF 8.097
Dongfang Wang,Guilong Zhang,Zhangyu Dai,Linglin Zhou,Po Bian,Kang Zheng,Zhengyan Wu,Dongqing Cai
In this work, a novel nanosystem with a sandwich-like structure was synthesized via face-to-face combination of two pieces of waste cotton fabrics (CFs) carrying ferrous sulfide (FeS) and carboxyl-functionalized ferroferric oxide microsphere (CFFM), respectively, and the obtained nanosystem was named as FeS/CFFM/CF. Therein, FeS has high reduction and adsorption capabilities for hexavalent chromium (Cr(VI)), CFFM possesses a high adsorption ability on cadmium ion (Cd(II)) through electrostatic attraction and chelation, and CF displays high immobilization ability for FeS and CFFM and adsorption performance on Cd(II). FeS/CFFM/CF could simultaneously remove Cr(VI) and Cd(II) from water and inhibit the uptake of Cr and Cd by fish and water spinach, ensuring the food safety. Besides, this technology could efficiently control the migration of Cr(VI) and Cd(II) in the sand–soil mixture, which was favorable to prevent their wide diffusion. Importantly, FeS/CFFM/CF possessed a high flexibility and could be conveniently produced with needed scale and shape and easily separated from water and soil, displaying a promising approach to remediate Cr(VI)-/Cd(II)-contaminated water and soil and a huge application potential.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Liqing Zhang,Bo Li,Zhenye Jiang,Haoyuan Xu,Chengqian Li,Yonggang Wei,Hua Wang
Among many pollution sources, Cr(VI) has captured much attention because of its strong toxicity, bioaccumulation and carcinogenicity. In recent years, nanoscale magnesium oxide has shown great potential in removing Cr(VI) pollution in water by virtue of its excellent adsorption and environmental friendliness. In this study, a high‑magnesium slag produced during the nitric acid pressure leaching process of laterite nickel ore was utilized as raw material for nano MgO preparation. A nano MgO-based adsorbent material (T-MgO) was prepared via the modification of MgO by nano TiO 2 which was synthesized use low-grade titanium slag as titanium source. Adsorption results demonstrated that T-MgO exhibits rapid adsorption performance, reaching adsorption equilibrium within 60 min. The kinetic adsorption conforms to the pseudo-second-order (PSO) model, revealing a chemisorption-dominated mechanism. According to the Freundlich model analysis, saturated adsorption capacity of the T-MgO for Cr(VI) reached 241.53 mg/g. The T-MgO material also possesses excellent reusability and selectivity to Cr(VI) adsorption. Furthermore, an in-depth analysis was performed to elucidate the Cr(VI) removal mechanism. Cr(VI) existing as HCrO 4 − and Cr₂O₇ 2− species under pH = 2 is electrostatically adsorbed on the protonated active sites of T-MgO. With the participation of free electrons generated by the nano-TiO 2 semiconductor, Cr(VI) is reduced to low-toxicity Cr(III), forming Mg-O-Cr bonds. The study achieved the purposes of superior and economic removal of Cr(VI) and high value-added utilization of the magnesium and titanium secondary resources.
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