JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Shuang Xu,Lijun Li,Zhaoliang Yu,Xiaodong Dai,Shuyan Yu,Congju Li
M/N/C-based single-atom catalysts (SACs) attract significant attention for oxygen reduction reactions (ORR), with Fe-Nx SACs demonstrating the highest activity. However, the Fenton reaction between iron-based catalysts and H 2 O 2 causes carbon matrix oxidation and corrosion, leading to stability issues. In this work, ZIF-8 serves as a substrate for anchoring Cr atoms, producing Cr-Nx/C SACs with low Fenton reaction activity through pyrolysis. To enhance Cr-Nx activity and further suppress the Fenton reaction, the carbon matrix is carefully engineered. Electrospinning technology uniformly distributes Cr-Nx/C as a functional structure on carbon nanofibers, resulting in Cr-Nx/C@CNF SACs. During pyrolysis, Zn volatilization from ZIF-8 generates numerous mesoporous structures that precisely connect to the catalytic active sites. The spatial network structure formed by the carbon nanofibers further contributes to the hierarchical porous carbon nanostructure of Cr-Nx/C@CNF SACs. The optimized Cr-Nx/ [email protected] catalyst exhibits excellent ORR activity, with a half-wave potential of 0.739 V vs. RHE. More importantly, the introduction of Cr-Nx and the optimized carbon matrix effectively suppress the Fenton reaction, improving stability. Furthermore, microbial fuel cells (MFCs) using Cr-Nx/ [email protected] as the cathode catalyst achieve a power density of 674.98 mW/m 2 and demonstrate superior durability, outperforming commercial Pt/C catalysts.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Ming Zhang,Qingkai Shi,Jing Tong,Min Cheng,Hao Ge,Sai Li,Guangfu Wang,Li Du,Hongda Liu,Ao Chen,Zhongwu Li
Based on Cr(VI) reduction, organic pollutants oxidative degradation and the excellent properties of carbon materials, the effectiveness of carbon materials for enhanced simultaneous Cr(VI) reduction and organic pollutants removal was verified. In this work, reduced graphene oxide (rGO) showed high catalytic activity, achieving > 99 % removal of both 10 mg/L 4-methoxyphenol (MOP) and 0.075 mM Cr(VI) within 20 min (k obs of 0.1723 min −1 and 0.1688 min −1 , respectively). To analyze the structure-activity relationship of the carbon materials in the system, a series of rGO derivatives were prepared. The results showed that the redox efficiencies of MOP and Cr(VI) had a significant positive correlation with the defect level of rGO, while the oxygen content was a negative factor for the catalytic performance, demonstrating that the defects were the main sites mediating the redox of MOP and Cr(VI). Furthermore, the O 2 • − , 1 O 2 and electron transfer pathway were identified as the mechanisms of MOP degradation and Cr(VI) reduction, according to quenching, electron spin resonance, salt-bridging and electrochemical oxidation experiments. Ultimately, the stability, broad applicability of simultaneous redox of MOP and Cr(VI) mediated by rGO were confirmed by cycling experiments, degradation experiments in various waters and with different pollutants. This study provides new mechanistic insights for the synergistic treatment of composite pollution using carbon materials.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2025
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IF 4.9
Nannan Huang,Shuhao Liang,Xiangyang Liang,Huining Chai,Yingjie Sun,Lili Lyu,Weiqiang Tan
The interfacial compatibility of heterojunction photocatalysts critically governs the interaction modes between constituent materials. Herein, a flower-like Bi-BDC-NH 2 /Ag 2 CO 3 heterostructure was fabricated via a simple ion-exchange solution method, serving as a robust photocatalyst for the efficient photocatalytic reduction of Cr(VI) in simulated wastewater under visible-light irradiation. Ag 2 CO 3 nanosheets were in-situ grown on the surface of three-dimensional Bi-BDC-NH 2 , forming an Ag 2 CO 3 -on-Bi-BDC-NH 2 type II heterojunction that establishes intimate interfacial contact, significantly accelerating the charge and mass transport dynamics. In comparison with pure Bi-BDC-NH 2 and Ag 2 CO 3 , the optimal Bi-BDC-NH 2 /Ag 2 CO 3 -50 (with a weight ratio of 0.5:1) exhibited dramatically enhanced photocatalytic activity, achieving 99% Cr(VI) reduction within 2 hours under visible light (>420 nm, 150 W xenon lamp). Mechanistic investigations, including energy band structure analysis, radical trapping experiments, and photoelectrochemical measurements, revealed that the heterojunction interface significantly promotes the separation and transfer of photogenerated electron-hole pairs. This work provides valuable insights into the rational design of MOF-based heterojunction photocatalysts and their applications in environmental remediation.
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CHEMICAL GEOLOGY
·
2025
·
IF 3.6
Changjin Liang,Honghai Wu,Yaowei Li,Yufeng Guan
Ferrihydrite (Fh) can usually transform into phases with higher crystallinities. This may greatly alter Fh adsorption capacity for chromium ions, thereby affecting their immobilizations and fates. Foreign elements [e.g., lanthanum (La)] as impurities can become incorporated into Fh. Herein, the effect of La-substitution into Fh and the influence of the presence of Cr(VI) on Fh phase transformation and fate of Cr(VI) were investigated. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Electro-chemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS) and other test methods were employed to probe phase changes after the Fe(II)-induced La-substituted Fh (La-Fh) transformations. At pH 5.5, no neoformed phase was observed until 7 d for La-Fh or pure Fh at 1 mM Fe(II) aq, but all La-Fh systems underwent transformations at 5 mM Fe(II)aq. A low pH and Fe(II)aq level favored lepidocrocite (Lp) to form, whereas goethite (Gt) was the predominant phase rather than Lp as pH increased to 7.2 with higher level Fe(II)aq. However, the La-substitution inhibits the La-Fh transformation rate and path. This made 5 % La-Fh transformed to Lp after 30 d at pH 7.2 and 1 mM Fe(II)aq. The La-release was present to some extent during the transformation process. Either the inhibition to La-Fh transformation or the La-slow release favors the retention of early-adsorbed Cr(VI) on iron-mineral surface. The added Cr(VI) might promote the La-Fh transformation even under a lower-level Fe(II), primarily attributed to the rapid reduction of Cr(VI) to Cr(III) by Fe(II), which produced more liable Fe(III) in addition to the Cr(III) that can improve the mineral conductivity, thereby enhancing the La-Fh transformation. Mechanisms responsible for the Fe(II)-induced La-Fh transformation companying the La slow-release are proposed to provide insights into the reduction and immobilization of Cr(VI) under anaerobic conditions, thus demonstrating that La-Fh is a promising material for application in Cr-contaminated site remediation.
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Separations
·
2025
·Vol. 12
·期 9
·247
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IF 2.7
Na Huang,Shengwen Chen,Wanhe Du
The photocatalytic reduction of hexavalent chromium (Cr(VI)) in wastewater represents a critical environmental challenge, given its high toxicity and mobility in wastewater. Conventional optimization methods relying on repetitive batch experiments with excessive reagent consumption. Herein, we proposed a synergistic experimental–deep learning approach to realize efficient photocatalytic reduction of Cr(VI). Sludge and cellulose precursors were used to prepare N-doped porous carbon through a green fabrication method at low temperature. After optimizing the composition and experimental factors, the removal efficiency of Cr(VI) could reach 92.7% after visible light irradiation in an acidic environment. The high efficiency originated from the coupled adsorption and photocatalytic mechanism. Innovatively, after comparing three algorithms, TCN and Transformer were employed to predict the desirable removal efficiency with <5% prediction error under different reaction conditions. This work highlights the novel experimental–deep learning method for heavy metal remediation using N-doped waste-derived porous carbon.
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Science Bulletin
·
2025
·
IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Fen Zhang,Shuyu He,Luyao Xi,Liying Ma,Liwen Zhang,Ling Xiong,Shaohua Chen,Benjun Xi
Reduction of Cr(VI) to Cr(III) or elimination of Cr(VI) from aqueous environments is the most commonly used method to address Cr(VI) contamination. Waste molasses (WM) is a by-product from the sugar industry, if discharged arbitrarily without treatment can lead to waste of resources and cause serious environmental pollution . In this study, the modification of polypyrrole (PPy) with WM (PPy/WM) not only provided PPy with good dispersibility and higher specific surface area, but it can also enrich the functional groups on the surface of PPy. The findings indicated that PPy/WM composites can serve as superior adsorbent materials for highly efficient and selective removal of Cr(VI) when different interfering ions are present. e.g., 150 mg/L of Cr(VI) can be eliminated completely within 6 h under the condition of PPy/WM amount of 0.8 g/L, temperature of 303 K, and pH of 2.0. PPy/WM showed excellent performance for removal of Cr(VI) in a wide pH range (2.0 - 10.0). PPy/WM exhibited excellent reusability for five cycles without obvious loss of its adsorption capacity. The maximum Cr(VI) adsorption capacity of PPy/WM was 662.25 mg/g at 323 K, evidently higher than that of unmodified PPy (194.17 mg/g). Cr(VI) removal by PPy/WM was chiefly accomplished by electrostatic adsorption, ion exchange and in-site reduction. This study not only provides a new technology for efficient adsorption and in-situ reduction of Cr(VI), but also realizes the resource utilization of WM and solves the WM pollution problems.
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MOLECULES
·
2024
·Vol. 29
·期 14
·3417
·
IF 4.2
Pengfei Zhu,Zhaoxia Hu,Shouwen Chen
The development of economical catalysts that exhibit both high activity and durability for chlorinated volatile organic compounds (CVOCs) elimination remains a challenge. The oxidizing and acidic sites play a crucial role in the oxidation process of CVOCs; herein, praseodymium (Pr) was introduced into CrOx catalysts via in situ pyrolysis of MIL-101(Cr). With the decomposition of the ligand, a mixed micro-mesoporous structure was formed within the M-Cr catalyst, thereby reducing the contact resistance between catalyst active sites and the 1,2-dichloroethane molecule. Moreover, the synergistic interaction between chromium and praseodymium facilitates Oβspecies and acidic sites, significantly enhancing the low-temperature catalytic performance and durability of the M-PrCr catalyst for 1,2-dichloroethane (1,2-DCE) oxidation. The M-30PrCr catalyst possess enhanced active oxygen sites and acid sites, thereby exhibiting the highest catalytic activity and stability. This study may provide a novel and promising strategy for practical applications in the elimination of 1,2-DCE.
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Analytical Methods
·
2024
·
IF 2.7
Taohong Zhou,Jin Lin,Fengmei Jin,Yanxing Yao,Zhihao Li,Lihua Wang
Cr(VI) is one of the most typical heavy metal contaminants and rapid detection of Cr(VI) is highly important in food control and public health. Herein, a core–shell Au@Pt nanozyme-based colorimetric assay was developed for the rapid and sensitive detection of Cr(VI). The monodispersed Au@Pt core–shell nanoparticles exhibited high peroxidase-mimicking activity and can catalyze colorless TMB into blue-colored oxidized oxTMB. After the addition of Cr(VI), the oxTMB molecules can be reduced into colorless TMB. The ultrathin Pt shell can prevent the Pt component from aggregation, thus improving the catalytic activity of Au@Pt nanozyme. These Au@Pt nanozyme-based Cr(VI) assays exhibited high sensitivity and selectivity and displayed satisfactory recoveries in practical samples. Our work highlights opportunities for the development of core–shell nanozymes with extensive applications in food safety, biomedicine, and environmental monitoring.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Hanqing Yu,Shijiao Li,Zheng Zeng,Guangxu Yang,Xu Tang,Yujia Zhang,Yi Dai,Lingyun Zhou,Xin Tong,Yadian Xie
The contamination of water with hexavalent chromium (Cr(VI)) poses a significant environmental and health threat. Basalt fiber (BF) is a high-strength, high-temperature-resistant, corrosion-resistant, and eco-friendly inorganic fiber material that shows promise for addressing such contamination. However, a key challenge lies in how to effectively modify its surface functionality and enhance the overall performance of fiber composites to improve adsorption efficiency, especially in large-scale applications. In this study, we present a scalable fabrication method for graphene-basal composite material using a layer-by-layer deposition technique. This process enables the mass production of highly efficient Cr(VI) adsorbents. It exhibited a Cr(VI) removal rate of up to 97.9 % within 2 h, making it a promising candidate for efficient Cr(VI) adsorption. The composite material, integrating the high surface area of graphene with the mechanical strength and chemical stability of basalt, exhibits superior adsorption capacity and reusability in removing Cr(VI) from contaminated water. Density functional theory (DFT) calculations indicated that the synergistic interaction between GO and BF enhanced both the physical and chemical adsorption of Cr(VI), facilitating its removal. Batch experiments demonstrate that the composite achieves rapid and efficient Cr(VI) removal across a wide range of pH levels and initial concentrations. The simple and scalable fabrication process highlights the potential for practical applications in large-scale water treatment. Furthermore, this study provides insight into the mechanisms underlying the adsorption process, offering a sustainable, rapid, and cost-effective solution to heavy metal pollution in environmental water bodies.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Wenhao Wang,Xingyu Wang,Xuechen Wu,Jinhua Zhang,Hejie Qin,Jinxiang Li
Nanoscale zerovalent iron (nZVI) has been extensively applied in water pollution control. However, the reactivity of nZVI toward contaminants is mainly limited by its corrosion and agglomeration. In this study, the nZVI modified by sulfidation coupled with carboxymethyl cellulose (CMC) (C-S-nZVI) was synthesized and characterized by TEM and electrochemical techniques. Taking Cr(VI) as the contaminant, it was found that the sulfidation could couple with CMC modification to not only enhance the reactivity of nZVI toward Cr(VI), but also regulate the sedimentation activity and corrosion activity of nZVI in water. Particularly, the optimal k obs (0.0816 min −1 ) obtained by the C-S-nZVI one -0.16 (i.e., one-step sulfidation and its S/Fe molar ratio was 0.16) was approximately 27.2 times higher than that by the nZVI (0.0030 min −1 ). Moreover, based on the correlation analysis of the ternary activities, this study confirmed that the reactivity of C-S-nZVI toward Cr(VI) was negatively correlated with its sedimentation activity (slope = −0.7623, R = 0.59) and corrosion activity (slope = −0.0171, R = 0.56), respectively. XPS and TEM results further revealed that CMC could couple with iron sulfides (FeS x ) to enhance the mass transfer of Cr(VI) toward nZVI and subsequent electron transfer from Fe 0 core to out, ultimately improving the reduction of Cr(VI) by nZVI. Overall, this study introduced a new evaluation method based on the ternary activity of nZVI, providing theoretical support for the practical application of nZVI-based technology.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Qian Zhou,Derong Liu,Guoyuan Yuan,Yi Tang,Kuncheng Cui,Songshan Jiang,Yongde Xia,Wei Xiong
Novel Ti/PbO 2 -Cr-PEDOT electrodes were prepared by electrodeposition for electrochemical degradation of phenolic wastewater. The electrodes were characterized by XRD, SEM-EDS, XPS, and FT-IR to study the crystalline, surface morphology, elements distribution, and microstructure of the electrodes. A flat and compact interface was obtained with Cr and PEDOT doping into β-PbO 2 plate by electrodeposition method. The linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) were conducted to explore the electrochemical performance of the prepared electrodes. The Ti/PbO 2 -Cr-PEDOT electrode exhibited a higher oxygen evolution potential (OEP, 2.53 V vs SCE) and a lower charge transfer resistance compared with Ti/PbO 2 . Phenol degradation efficiency of 100% and TOC removal rate of 95.02% were achieved in the electrochemical degradation of phenol within 120 min. The optimal process parameters (phenol concentration = 1000 mg·L -1 , electrolyte concentration = 4.0 g·L -1 , current density = 15 mA·cm −2 and electrode distance = 3 cm) in the process of electrochemical oxidation of phenol wastewater were explored. Active species trapping experiments proved that ·OH radicals played an important role in the electrochemical system. Furthermore, the electrode also showed high activity for the degradation of other phenolic wastewaters such as phloroglucinol (η DEP = 100%), bisphenol A (η DEP = 97.17%) and p-chlorophenol (η DEP = 89.77%) within 60 min. A possible degradation pathway was proposed based on the intermediate products determined by HPCL. The Ti/PbO 2 -Cr-PEDOT electrode showed excellent stability with only 3% loss of degradation efficiency (η DEP = 96.95%) after recycling tests for 5 times. These results suggest that Ti/PbO 2 -Cr-PEDOT is a promising electrode for electrochemical degradation of phenolic wastewaters.
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