JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Enjie Wu,Jintao Zhou,Dianming Ren,Honggui He,Jingyu Pan,Chuqing Tang,Xupin Zhuang
Hexavalent chromium (Cr(VI)) contamination poses severe ecological risks due to its carcinogenicity and prevalence in industrial wastewater, where metal-organic frameworks (MOFs) show photocatalytic remediation potential. However, powdered MOFs suffer from poor recyclability and secondary pollution risks in practical applications. This study proposes an integrated structural-interfacial engineering strategy that combines the design of a robust three-dimensional fiber network framework with the interfacial engineering of MOFs and cellulose nanofibers to fabricate robust MOF-functionalized aerogel (MOFA) photocatalyst. The MOFAs feature hierarchical coordination effects enabling precise MOF crystallization control, achieving ultrahigh MOF loading (76.77 wt%), mechanical robustness (29 kPa stress at 70 % compression), exceptional stability (6.7 % permanent deformation after 100 cycles), and enhanced photocatalytic activity (photocurrent density of 2.87 μA/cm²). The optimized interfacial structure delivers superior adsorption (67 %) and photocatalytic performance (100 % Cr(VI) reduction in 80 min, > 94 % efficiency retention after 5 cycles), validated across diverse water matrices including high-salinity tanning wastewater under outdoor conditions. This innovative strategy offers a new design approach for developing high-performance photocatalytic materials and holds important application prospects in environmental governance.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yifei Yin,Wenjun Zhou,Ming Zhang
A microscale zero-valent iron (mZVI) composite integrating surface phosphate (P) modification and lattice nitrogen (N) doping (NP-mZVI) was successfully fabricated by one-step mechanochemical method in aim to establish synergistic adsorption-reduction pathways for enhanced Cr(VI) removal. NP-mZVI demonstrated superior reactivity for Cr(VI) removal with 100% of both removal efficiency and conversion rate, which significantly outperform the pristine ball-milled mZVI bm and P-modified mZVI bm . Furthermore, NP-mZVI also exhibited excellent removal performance for a range of heavy metals (e.g., Ni(II), Pb(II), Cu(II), and Cd(II)), and was also demonstrated to be pH-universal, long-term stability, and environmental applicability. The strategic integration of lattice N doping and surface P coordination in NP-mZVI establishes a dual-path optimization mechanism for enhanced Cr(VI) removal. Surface P groups enable bidentate Cr(VI) complexation through ligand-specific recognition, reducing adsorption energy barriers while creating Fe-O-P mediate directional charge transfer. Concurrently, interstitial N doping induces lattice tensile strain via Fe Fe bond elongation, weakening metallic bonding networks to amplify electron liberation from the Fe 0 core. N facilitates electron release through strain engineering while P directs interfacial electron utilization. This synergistic coupling of core activation and surface mediation resolves the kinetic mismatch between electron supply and interfacial demand, achieving superior Cr(VI) removal efficiency through adsorption-reduction pathway integration. This study highlighting the synergistic effects of surface P modification and lattice N doping for mZVI in enhancing the reduction and removal of Cr(VI), and provides a new insight into rational design of modified mZVI with high reactivity.
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Molecular Catalysis
·
2026
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IF 4.3
Chuanhua Li,Yubao Shi,Linxia Chen,Ziheng Wang,Wei Xiao,Xuemin Yan
Electrolysis of water to produce hydrogen can alleviate the problem of global energy shortage, and seeking efficient water splitting electrocatalysts is the promising direction. In this work, Cr-doped nickel oxalate (Cr-NiC 2 O 4 /NF) was synthesized on nickel foam (NF) by a one-step hydrothermal method and used as an alkaline electrolytic water catalyst. The electrocatalytic activity of NiC 2 O 4 is significantly improved by Cr doping. For the oxygen evolution reaction (OER), the overpotential is 324 mV at 100 mA cm -2 , and for the hydrogen evolution reaction (HER), the overpotential is 191 mV at 10 mA cm -2 . When Cr-NiC 2 O 4 /NF is used as anode and cathode in water splitting, only voltage of 1.58 V is required at current density of 10 mA cm -2 . Furthermore, the mechanism of enhanced catalytic activity via surface reconstruction during the OER and HER was systematically studied. The pre-catalyst Cr-NiC 2 O 4 was restructured into hydroxides and hydroxyl oxides for OER, and some Cr-NiC 2 O 4 was converted into hydroxides for HER. Consequently, this investigation provides a new method to improve the electrocatalytic performance of metal oxalates and a theoretical guidance for surface reconstruction.
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Chemical Science
·
2026
·
IF 7.4
Jiahe Li,Gaili Ke,Minji Yang,Guoliang Lv,Lanyi Cao,Wenjun Li,Tao Han,Wenrong Wang,Yong Zhou,Huichao He
The presence of Cr defects in monoclinic PbCrO4 is closely related to its solar water oxidation activity, which be overlooked in the preparation of PbCrO4 films and unrevealed in the researches of PbCrO4 photoanodes. Herein, monoclinic PbCrO4 films with few Cr defects (PbCrO4-FVCr) were prepared on FTO substrate through covering the drop-coating Pb2+/Cr3+ precursor solution to reduce the loss of Cr during thermal treating. Relative to the monoclinic PbCrO4 films with rich Cr defects (PbCrO4-RVCr), higher solar water oxidation activity was achieved on the PbCrO4-FVCr films as photoanodes. At 1.23 V vs. RHE, a higher water oxidation photocurrent of 1.13 mA cm-2 was produced on the PbCrO4-FVCr film photoanodes, which is two-fold to the PbCrO4-RVCr film photoanodes (0.55 mA cm-2). Meanwhile, the PbCrO4-FVCr film photoanodes had faster water oxidation kinetics than PbCrO4-RVCr film photoanodes. The water oxidation rate constant (kO2) on the PbCrO4-FVCr film photoanodes was 40.6 s-1, while a lower kO2 of 8.2 s-1 on the PbCrO4-RVCr film photoanodes. Experimental detections and theoretical calculations jointly revealed that PbCrO4 films with fewer Cr defects being of higher solar water oxidation activity can be attributed to following reasons: (i) the presence of Cr defects can result in the formation of deep energy level in PbCrO4, which is unfavorable to carrier transfer in the bulk of PbCrO4 films; (ii) the presence of Cr defects can cause the formation of unsaturated O dangling bonds on PbCrO4, which are harmful traps for carrier separation on the surface of PbCrO4 films; (iii) Cr has a half-filled 3d5 orbital to provide active sites for reaction, the presence of Cr defects weakens the catalytic activity of PbCrO4 for water oxidation, and turns the rate-limiting step to the dehydrogenation of *OH into *O which requires a high energy barrier of 1.88 eV. The present work provides insight into monoclinic PbCrO4 film photoanodes from the relevance of preparation condition, Cr defects, water oxidation activity and reaction mechanism.
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WATER SCIENCE AND TECHNOLOGY
·
2020
·Vol. 82
·期 3
·492-502
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IF 1.638
Wei Jinyu,Hu Huayu,Zhang Yanjuan,Huang Zuqiang,Liang Xingtang,Yin Yanzhen
In this work, a user-friendly chitin-based adsorbent (CT-PmPD) was synthesized by in-situ polymerization of m-phenylenediamine on chitin bead, which could effectively remove Cr(VI) from water. The structure and morphology of the CT-PmPD were characterized by FT-IR, XRD, SEM, zeta potential and XPS. Specifically, the effect of adsorbed dosage, pH, contact time, adsorption temperature and coexisting salt on the adsorption of Cr(VI) were studied. Besides, the adsorption mechanism of CT-PmPD toward Cr(VI) were also analyzed. Consequently, CT-PmPD exhibited a monolayer adsorption and the Langmuir model fitted a Cr(VI) adsorption capacity reaching 185.4 mg/g at 298 K. The high adsorption capacity was attributed to the abundant amino groups of CT-PmPD, which could be protonated to boost the electrostatic attraction of Cr(VI) oxyanions, thus providing electron to reduce Cr(VI). Additionally, the CT-PmPD revealed a good regeneration and reusability capacity, maintaining most of its adsorption capacity even after five cycles of adsorption-desorption. This high adsorption capacity and excellent regeneration performance highlighted the great potential of CT-PmPD for the removal of Cr(VI).
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CHEMICO-BIOLOGICAL INTERACTIONS
·
2026
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IF 5.4
Yuankun Zhou,Jiajun Guo,Xiaoyan Feng,Hengyi Xu
Nanoplastics (NPs) and chromium (Cr) are ubiquitous in the environment, causing severe pollution and posing significant potential threats to human health. Polylactic acid (PLA) and Cr are among widely used bioplastic and heavy metal, respectively, both capable of contaminating water sources through corresponding pathways and posing substantial risks to human health. Nanoplastics can act as carriers for heavy metals, thereby enhancing their bioaccumulation and toxicity. Therefore, this study investigated the effects of combined exposure to Cr(VI) and PLA NPs on mice kidneys and its potential mechanisms. Results indicated that exposure to PLA NPs alone did not exhibit significant toxic effects on the kidneys. However, combined exposure to Cr(VI) and PLA NPs caused severe kidney damage in mice. This indirectly suggests that Cr(VI) and PLA NPs exhibit synergistic toxicity rather than simple additive effects. Furthermore, combined exposure exacerbated the toxic mechanism by inducing mitochondrial damage and excessive reactive oxygen species (ROS) production, thereby triggering mitophagy. Overactivated mitophagy exacerbated lipid peroxidation by releasing free iron, thereby amplifying ROS-mediated ferroptosis. This study investigates the synergistic renal toxicity of Cr(VI) and PLA NPs, providing scientific evidence for the combined toxicity mechanism of exposure to MNPs and heavy metals.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jianle Wang,Xueming Liu,Hong Deng,Dongye Zhao,Qiulin Yang,Zhihua Zhu
Various sulfur- and iron-bearing materials have been shown promising for reductive immobilization of Cr(VI) in water and soil. Yet, composite Ca-Fe-S materials and the effects of water chemistry and material aging have not been investigated. In this work, we prepared a type of Ca-Fe-S microparticles under the atmospheric conditions through a facile one-pot approach, and tested the particles for reductive immobilization of Cr(VI) in solution and soil. Ca-Fe-S showed 40 % higher removal efficiency of Cr(VI) in solution than FeSO 4 and 10 % higher than CaS x on the basis of equal molar dosage. When a Cr-laden soil was amended by Ca-Fe-S, the leachable concentration of Cr per the toxicity characteristic leaching procedure remained below the regulatory limit of 5 mg L −1 after 730 days of curing, while FeSO 4 and CaS x failed to meet the regulatory threshold. Ca-Fe-S served as a slow-releasing source of Fe 2+ and S 2- , which were able to convert Cr(VI) into the stable final product of Cr(OH) 3 . Ca-Fe-S was able to perform well under a wide range of pH (3.0–9.0) and in the presence of high concentrations of coexisting ions (5 mmol L −1 of Cl - , SO 4 2- , or HCO 3 - ). Moreover, the material remained effective when aged under the atmospheric conditions for 14 days. This study showed that Ca-Fe-S is a highly effective material for efficient sequestration of Cr(VI) in soil and groundwater under various water chemistry and materials aging conditions.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Shengwen Wang,Yu Shi,Hao Zhang,Yufeng Sun,Fangfang Wang,Leyong Zeng,Xing Li,Aiguo Wu,Yujie Zhang
Hexavalent chromium (Cr(VI)) is highly carcinogenic and mutagenic, which is seriously harmful to human health. Hence, it is important to create a probe that can detect Cr(VI) effectively. In this work, gold nanotetrapods (Au NTPs) were applied in colorimetric detection for the first time. Based on the oxidative etching principle of Cr(VI) on Au NTPs, a sensitive and multicolor response detection method for Cr(VI) was established. The oxidative etching of Au NTPs by Cr(VI) resulted in the blue shift of plasmon resonance absorption peak of Au NTPs with the change of morphology. As the etching progress processed, Au NTPs solution exhibited obvious color changes from gray-green to blue-violet and then to pink. This multicolor response design is very convenient for naked-eye detection. The limit of detection (LOD) of Cr(VI) is 3 nM for the naked eyes and 0.5 nM for UV–vis spectrum, both of which are lower than the toxicity level of Cr(VI) (0.2 μM) set by United States Environmental Protection Agency. This sensing method exhibits good linearity between the wavelength shift and Cr(VI) concentration in the range of 0.5 nM to 8 nM. The detection results of Cr(VI) in actual environmental samples demonstrate that the Au NTPs colorimetric probe (Au-N-Probe) is expected to be applied to the detection of Cr(VI) in water environmental samples such as lake water and industrial wastewater.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yu-Fei Li,Can-Jun Zou,Xing-Biao Liu,Feng Gan,Ping-Ping Fang
The detection of pharmaceuticals has been a matter of concern among scientists and health researchers in the past few decades. However, it is still difficult to realize the sensitivity and selectivity detection of pharmaceuticals with similar structures. Herein, the pharmaceutical molecules of 2-mercaptobenzimidazole (MBI) and 2-mercaptobenzothiazole (MBT) with so similar structures can be selectively detected by surface-enhanced Raman spectroscopy (SERS) taking advantage of the fingerprint identification on Au/MIL-101(Cr), with sensitive detection limits of 0.5 ng·mL–1 for MBI and 1 ng·mL–1 for MBT. MBI is selectively enriched by Au/MIL-101(Cr) from the mixture solution and detected by SERS below 30 ng·mL–1. MBI can also be selectively detected in the serum samples with a detection limit of 10 ng·mL–1. Density functional theory calculations combined with the SERS experiments explained that the high sensitivity and selectivity are caused by the intrinsic differences in Raman intensity and different adsorption energies from the pharmaceutical molecules adsorbed on Au/MIL-101(Cr), respectively. This study provides an effective way to enrich and detect pharmaceutical molecules with similar structures.
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Catalysts
·
2023
·Vol. 13
·期 5
·876
·
IF 3.9
Huan He,Xusheng Wang,Qin Yu,Wenbin Wu,Xinya Feng,Deyu Kong,Xiaohui Ren,Junkuo Gao
Cr(VI) is one of the most toxic heavy metals, posing multiple threats to humans and ecosystems. Photoreduction of toxic Cr(VI) to para-toxic Cr(III) is one of the most effective ways to remove heavy metal chromium but is still challenging. Herein, Ti3C2/UiO-66-NH2composites with different ratio of Ti3C2were synthesized via an in situ solvothermal process and used for the enhanced photocatalytic removal of Cr(VI) for the first time. The UiO-66-NH2nanoparticles were dispersed on the surface and slits of accordion-like Ti3C2homogeneously. A strong interfacial interaction between Ti3C2and UiO-66-NH2was formed, which was indicated by the XPS. The Fermi level of the MXene cocatalyst is lower than UiO-66-NH2; thus, Ti3C2can serve as the electron sink and accumulate photogenerated electrons from UiO-66-NH2on its surface. A depletion layer was also formed due to the different Fermi levels of UiO-66-NH2and Ti3C2, which prevents electrons from flowing back to UiO-66-NH. The strong interfacial interaction and formed depletion layer are beneficial for the following charge transfer from UiO-66-NH2to Ti3C2after light irradiation and for suppressing the photogenerated charge recombination. With suitable band positions and enhanced charge separation ability, Ti3C2/UiO-66-NH2composites exhibited better photoreduction efficiency of Cr2O72−than pure Ti3C2and UiO-66-NH2, with optimized samples reaching 100% in 40 min. The photoreduction kinetics of Cr2O72−by 2-T/U was also studied, with a photoreduction rate of 0.0871 min−1, which is about 2.6 times higher than that of the pure UiO-66-NH. This research provides a new type of efficient and environmentally friendly photocatalysts for the photoreduction of Cr2O72−.Keywords:metal–organic frameworks;photocatalysis;MXene;Cr(VI);photocatalyst;photoreduction;porous materials
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Materials
·
2023
·Vol. 16
·期 11
·3994
·
IF 3.4
Qingxiang Wang,Yan Yue,Wenfei Liu,Qing Liu,Yu Song,Chengjun Ge,Hongfang Ma
Biochar can be used to address the excessive use of tetracycline and micronutrient chromium (Cr) in wastewater that potentially threatens human health. However, there is little information about how the biochar, made from different tropical biomass, facilitates tetracycline and hexavalent chromium (Cr(VI)) removal from aqueous solution. In this study, biochar was prepared from cassava stalk, rubber wood and sugarcane bagasse, then further modified with KOH to remove tetracycline and Cr(VI). Results showed that pore characteristics and redox capacity of biochar were improved after modification. KOH-modified rubber wood biochar had the highest removal of tetracycline and Cr(VI), 1.85 times and 6 times higher than unmodified biochar. Tetracycline and Cr(VI) can be removed by electrostatic adsorption, reduction reaction, π–π stacking interaction, hydrogen bonding, pore filling effect and surface complexation. These observations will improve the understanding of the simultaneous removal of tetracycline and anionic heavy metals from wastewater.
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Molecular Catalysis
·
2022
·
IF 5.089
Rongzhao Li,Chengtao Zhang,Shuo Li,Yupeng Du
Propane dehydrogenation is commonly operated at temperatures exceeding 600 °C due to thermodynamic requirements. However, high temperature accelerates the deactivation of catalysts because of the coke deposition. Therefore, it is quite necessary to develop catalysts with high catalytic activity and improved anti-coking ability. To this end, an Al-doped Cr 2 O 3 catalyst derived from MIL-101(Cr/Al) is prepared in this work. The preparation conditions, including the carbonization temperature of MIL-101 and the proportion of Cr/Al, are optimized via experimental studies. Meanwhile, the adsorption and dehydrogenation behaviors of propane on the catalyst are investigated using Density Functional Theory (DFT) methods. Findings indicate that the optimum carbonization temperature and Cr/Al proportion are 900 °C and 6:4, respectively. Under the reaction condition of P = 0.1 MPa, T = 580 °C and GHSV = 800 h −1 , the propane conversion and propylene selectivity on the Cr 6 /Al 4 catalyst are 19.5% and 92.0%, respectively. The activity stability of the Al-doped Cr 2 O 3 is elongated significantly due to the lower desorption energy of propene and higher energy barrier for the coke formation on the catalyst. In sum, the present work completed via experiments and DFT calculations will lead to a better understanding of the Al-doped Cr 2 O 3 catalyst and guide the rational design of anti-coking catalysts for propane dehydrogenation.
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