CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ningyi Chen,Bingcai Pan
Toxic metal-organic complexes are ubiquitous in contaminated waters but more challenging than free ion counterparts for water decontamination. Currently, almost all the available analytical methods, including Au nanoparticles-mediated colorimetric assay, cannot discriminate metal-organic complexes from the total metal content, which greatly impedes the development of specific decontamination strategies for metal-organic complexes. In this study, we found that nitrilotriacetic acid (NTA) functionalized AuNPs could be used to determine various Cr(III) complexes (Cr(III)-lactate, Cr(III)-malonate, Cr(III)-oxalate, Cr(III)-tartrate, Cr(III)-citrate and Cr(III)-EDTA) in water. Mechanism study indicated that at acidic pHs (pH = 1.6), the protonation of organic ligands resulted in partial dissociation of Cr(III) from the corresponding complexes to expose its accessible orbitals for re-coordination with NTA. Such re-coordination induces the aggregation of the dispersed NTA-AuNPs and thereafter causes considerable changes both in color and UV–Vis spectrum of the solution. The nanosensor is highly selective to Cr(III)-organic complexes with detection limits of 0.029 μM for Cr(III)-lactate, 0.043 μM for Cr(III)-malonate, 0.35 μM for Cr(III)-oxalate, 0.079 μM for Cr(III)-tartrate, 2.58 μM for Cr(III)-citrate and 0.90 μM for Cr(III)-EDTA, respectively. The feasibility of the proposed colorimetric assay has been verified by using the authentic natural and industrial water samples. We believe this study will be of fundamental significance to push forward the application of Au NPs colorimetric assay in authentic waters contaminated by toxic metals.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Zhong-yi Wang,Rui-tang Guo,Zhen-zhen Guan,Xu Shi,Wei-guo Pan,Zai-guo Fu,Hao Qin,Xing-yu Liu
A sequence of Cr-modified CeZr 2 O x catalysts were synthesized through the co-precipitation way and applied in selective catalytic reduction (SCR) of NO x with ammonia. The optimal catalyst (Cr 1 CeZr 2 O x ) exhibited the excellent NH 3 -SCR activity and high SO 2 resistance. From the characterization results, Cr species in Cr 1 CeZr 2 O x could suppress the formation of ZrO 2 crystals, which could also contribute to stronger surface acidity and reducibility . Besides, more Ce 3+ and surface adsorbed oxygen species were observed on Cr 1 CeZr 2 O x catalyst. On the basis of in situ DRIFT experiments, it could be confirmed that the NH 3 -SCR process on Cr 1 CeZr 2 O x was promoted through Langmuir-Hinshelwood (L-H) mechanism. Besides, the improved NO oxidation and more ad-NO x and ad-NH 3 also played a vital role for the superior low-temperature SCR activity of Cr 1 CeZr 2 O x .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Quan Huo,Xiaoran Qi,Jianshu Li,Gongquan Liu,Yao Ning,Xubiao Zhang,Boyu Zhang,Yanfei Fu,Suyan Liu
A series of direct Z-scheme α-Fe 2 O 3 /MIL-101(Cr) hybrids were successfully prepared through a facile hydrothermal method in this work. And, the materials were characterized by some technologies including X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), N 2 adsorption-desorption, photoluminescence (PL) spectroscopy, Ultraviolet-visible (UV–vis) diffuse reflectance spectroscopy (DRS) and electron spin resonance (ESR). The photocatalytic activities of the hybrids were evaluated by degradation of carbamazepine (CBZ) under visible light irradiation. It is found that 100% of CBZ was able to be removed after 180 min irradiation over the optimum α-Fe 2 O 3 (0.3)/MIL-101(Cr) hybrid. The superior activity was engendered from good textural properties and the formation of a direct Z-scheme heterojunction in the hybrid. The decomposition process of CBZ and the formation of intermediate products were analyzed through liquid chromatography-tandem mass spectrometry (LC–MS) and a possible photodegradation pathway of the CBZ was proposed. Also, the possible mechanism for the photodegradation process was provided to illustrate the excellent performance. The work has paved a new way for the application of MOF materials in the design of efficient Z-scheme system for organic pollution degradation in wastewater.
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Environmental Science-Nano
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2025
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IF 5.1
Yanchun Liao,Wenhao Lao,Chenyi He,Junchun Li,Longyong Lin,Yiping Feng,Yirong Deng
Ferrihydrite (Fh), a metastable iron(oxyhydr)oxide abundant in soils and sediments, plays a pivotal role in regulating phosphorus bioavailability and contaminant Cr(VI) fate, but its rapid phase transformation to low-reactivity crystalline phases limits its long-term functionality. This study investigated how light (Nd3+) and heavy (Y3+) rare earth elements (REEs) modulate Fh's phase transformation and Cr(VI)/PO43− sequestration. The results showed that LREE Nd3+ predominantly adsorbed onto Fh surfaces, forming a protective layer that shielded reactive Fe–OH sites and delayed hydroxyl displacement. In contrast, HREE Y3+ underwent isomorphic substitution into Fh's octahedral Fe–O framework, inducing lattice distortion and suppressing acicular goethite crystallization by ca. 26%. Both REEs preserved Fh's metastability, and maintained Fe in the oxidized Fe3+ state. In addition, both Nd3+ and Y3+ integration into hematite during transformation slowed Fh conversion to low-adsorptivity crystalline phases. Consequently, after 30 days of aging, REE-doped Fh exhibited significantly enhanced Cr(VI)/PO43− sequestration (qmax,Cr(VI) = 19.39 mg g−1 and qmax,P = 43.33 mg g−1 for Fh–Nd, 24.47 and 64.03 mg g−1 for Fh–Y) compared to pristine Fh (qmax,Cr(VI) = 4.91 and qmax,P = 24.03 mg g−1). These enhancements might be driven by prolonged amorphous Fh persistence, REE–Cr(VI)/PO4 surface precipitation, and REE–O–Fe ternary binding sites. These findings clarify how REE–Fe coupling regulates Cr(VI)/PO43− fates in terrestrial ecosystems and also provide insights for designing REE-modified adsorbents for long-term contaminant/nutrient retention in soils or aquatic systems, where Fh's natural transformation would otherwise compromise such efficacy.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Biao Yuan,Pan Wu,Changjun Liu,Jian He,Wei Jiang
The challenge of separating and recovering V(V) and Cr(VI) from wastewater is critical for environmental protection and industrial productivity due to the chemical similarities. In this study, a novel zirconium-based adsorbent with superior adsorption performance and selectivity was synthesized using the Sol-Gel method, with a specific surface area of up to 265.3 m 2 /g. The maximum adsorption capacities of V(V) and Cr(VI) were 222 and 123 mg/g, respectively. The adsorption process followed the Langmuir isothermal adsorption and the pseudo-second-order kinetic model. The adsorption mechanism was thoroughly investigated confirming that the adsorption of V(V) and Cr(VI) on amorphous hydrous ZrO 2 (AHZOs) is chemisorption. At a pH of 3, the values of ΔG 0 (−46.8 kJ/mol) and E ads (−5.67 eV) for the main existing form H 3 V 10 O 28 3- on AHZOs are lower than those for the main existing form HCrO 4 - . V(V) replaced the adsorbed Cr(VI) during competitive adsorption to achieve selective adsorption of V(V) with a separation coefficient as high as 3142. The adsorption capacity of V(V) remains above 105 mg/g after five cycles. After adsorption, the purity of Cr(VI) can be increased to above 99.5 %, and a solution of V(V) with a purity higher than 99.25 % can be obtained after desorption. The use of 3 g/L and 100 g/L adsorbent can decrease the single V(V) and Cr(VI) to 1.618 mg/L and 0.36 mg/L, respectively, and meet the emission standards.
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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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Surfaces and Interfaces
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2024
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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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Science Bulletin
·
2025
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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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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
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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 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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高影响因子
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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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2015
·Vol. 17
·期 40
·26690-26702
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IF 4.493
Shengjie Xia,Mengmeng Shao,Xiaobo Zhou,Guoxiang Pan,Zheming Ni
A series of novel organic–inorganic nanoscale layered materials were synthesized by intercalating the Ti-containing Schiff base complex into the interlayer of the ZnM layered double hydroxides (LDHs, M = Al, Cr, Fe, Ce). The hybrid material was further calcined to make metal oxide composites with highly dispersed Ti elements (Ti/ZnO–MxOy). The structural characterization and photocatalytic results showed that, after intercalation and calcination, the metal oxide composites with a unique flower-like crystal morphology not only had high specific surface area, uniform pore size distribution and narrow band gap, but also showed extremely high photocatalytic performance for hexachlorobenzene (HCB) degradation. The Ti/ZnO–Cr2O3 composite with the narrowest band gap (2.40 eV) and the highest surface area (227 m2) showed the highest photocatalytic performance for HCB (95.5% within 240 min) among the four metal oxide composites. Particularly, it was found that composites derived from layered materials with different supramolecular structure of the host and guest showed different photocatalytic properties. In addition, based on the results from ESR, GC-MS and HPLC-MS, the type and amount of hydroxyl radicals, the decomposition intermediates and the pathway of HCB degradation photocatalyzed by Ti/ZnO–MxOy composites are also discussed in detail.
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