RSC Advances
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2024
·Vol. 14
·期 8
·5142-5148
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IF 3.9
Chunhong Jin,Jingchao Liu,Yilin Yin,Zenghe Li
In wastewater containing heavy metals, Cr(VI) is a potentially toxic metal, mainly derived from production and processing processes such as textile printing, dyeing, ore mining, battery applications, metal cleaning and electroplating. WO3 is widely used in photocatalytic degradation and reduction, and its utilization rate of visible light is high. However, the rapid recombination of photogenerated electron–hole pairs of WO3 limits its use. In this work, the composite material (WxMy) of WO3 and MIL-125 (Ti) was prepared by the ball milling method, and the catalyst was used to photocatalytically reduce Cr(VI). After using W90M10 as a photocatalyst for 50 min, the reduction rate of Cr(VI) can reach 99.2%, and the reduction rate is 2.3 times that of WO3. After 5 cycles of use, the reduction rate can still reach 91.3%. It is mainly due to the formation of a II-type heterojunction between WO3 and MIL-125 (Ti), which promotes the separation of photogenerated electron–hole pairs, thus improving the efficiency of photocatalytic reduction of Cr(VI).
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Cai Zhengwei,Liang Jie,Li Zixiao,Yan Tingyu,Yang Chaoxin,Sun Shengjun,Yue Meng,Liu Xuwei,Xie Ting,Wang Yan,Li Tingshuai,Luo Yongsong,Zheng Dongdong,Liu Qian,Zhao Jingxiang,Sun Xuping,Tang Bo
Electrocatalytic H 2 production from seawater, recognized as a promising technology utilizing offshore renewables, faces challenges from chloride-induced reactions and corrosion. Here, We introduce a catalytic surface where OH – dominates over Cl – in adsorption and activation, which is crucial for O 2 production. Our NiFe-based anode, enhanced by nearby Cr sites, achieves low overpotentials and selective alkaline seawater oxidation. It outperforms the RuO 2 counterpart in terms of lifespan in scaled-up stacks, maintaining stability for over 2500 h in three-electrode tests. Ex situ / in situ analyses reveal that Cr(III) sites enrich OH – , while Cl – is repelled by Cr(VI) sites, both of which are well-dispersed and close to NiFe, enhancing charge transfer and overall electrode performance. Such multiple effects fundamentally boost the activity, selectively, and chemical stability of the NiFe-based electrode. This development marks a significant advance in creating durable, noble-metal-free electrodes for alkaline seawater electrolysis, highlighting the importance of well-distributed catalytic sites.
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ENVIRONMENTAL RESEARCH
·
2025
·
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
·
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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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Lei Zhou,Xiayuan Yang,Xin Zhang,Mingzhe Li,Kepi Chen,Yuzhen Lv,Jin Zhang,Wei Zhou
It is of great significance to develop energy-saving and scalable synthetic methods for high-performance electrodes in green hydrogen production. Here we report a green room-temperature synthesis to produce integrated electrode with Cr-doped NiFe LDH/FeOOH nanosheets grown on iron foam. This simple one-step corrosion strategy can fabricate the electrode with an area up to 600 cm 2 . Through in situ self-activation process, the obtained Cr v -NiFeOOH/FeOOH@IF electrode exhibits excellent OER activity and durability, offering ultralow overpotentials of 279.3 and 308.4 mV to drive high current densities of 500 and 1000 mA cm −2 and operating steadily at industrial-level current density of 1000 mA cm −2 over 200 hrs with a high potential retention of 98.2 %. In situ electrochemical tests and theoretical calculations reveal the synergistic kinetics modulation. Both Cr vacancies and NiFeOOH/FeOOH heterostructure can accelerate water oxidation process by optimizing the adsorption energy of the intermediates. DFT calculations confirm Cr vacancies can further reduce the rate-determining step (RDS) energy barrier of the heterostructure. This work offers an economical and scalable corrosion strategy to produce high-efficient OER electrocatalysts toward industrial water splitting.
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CELLULOSE
·
2025
·
IF 4.8
Jin Mengyu,Wu Detong,Song Yuanbo,Shi Yang,Wang Xiaoxia,Shen Zheng,Zhang Yalei
This study presents an efficient strategy for converting high-boiling solvent (HBS) pretreated cellulose into lactic acid (LA) over a Cr-Sn-Beta bimetallic catalyst synthesized by flash Joule heating (FJH). Ethylene glycol-based HBS pretreatment effectively enriched cellulose content in straw, while the FJH method enabled rapid and uniform metal incorporation. The resulting Cr-Sn-Beta catalyst exhibited a maximum LA yield of 33.54% with a carbon balance of 90.08%, showing high selectivity and catalytic efficiency. The synergistic function of Cr and Sn acid sites was also evaluated. This work provides a promising route for biomass valorization and catalyst design via combined pretreatment and advanced synthesis techniques.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
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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INORGANIC CHEMISTRY
·
2024
·
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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Materials Today Communications
·
2024
·
IF 3.7
Chunlong Qiu,Haiyang Sun,Yeyang Ni,Zhenjiang Dou,Ming Xia,Zhaoyang Fei,Zhuxiu Zhang,Mifen Cui,Qing Liu,Xu Qiao
The impressive water stability demonstrated by MIL-101(Cr) highlights its considerable potential for the effective elimination of organic contaminants from wastewater. Nevertheless, the limited availability of adsorption sites within MOFs leads to an unsatisfactory capacity for tetracycline (TC) adsorption. In this case, the lanthanum modified MIL-101(Cr) porous adsorbents, termed as nLa-MIL-101(Cr), were successfully synthesized using a post-synthetic modification method. Through various characterization analyses, it was confirmed that lanthanum exists in the form of La(OH) 3 within the adsorbents, and all adsorbents also preserved the original structure as MIL-101(Cr). The results of static adsorption experiments demonstrated that, compared to the original material, the adsorption capacity of 1La-MIL-101(Cr) for TC increased by 3.5 times. Further experiments demonstrated that the adsorbent exhibits remarkable ion interference resistance and cycle stability. Finally, based on X-ray photoelectron spectroscopy, the adsorption mechanism was primarily attributed to the coordination between TC molecules and metals active site, while electrostatic interactions also played a significant role in the process. This study has developed a highly efficient adsorbent for the treatment of TC-contaminated wastewater, which reflects promising practical application prospects.
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Frontiers of Chemical Science and Engineering
·
2021
·Vol. 15
·期 5
·1185-1196
·
IF 4.204
Liu Wanyue,Liu Xiaoqin,Chang Jinming,Jiang Feng,Pang Shishi,Gao Hejun,Liao Yunwen,Yu Sheng
The magnetic nitrogen-doped carbon (MNC) was prepared from polypyrrole by a simple high temperature calcination process in this paper. The structure and properties of MNC were analyzed by scanning electron microscope, Fourier transform infrared spectroscopy, X-ray diffraction, Brunner-Emmet-Teller, vibrating sample magnetometer, and X-ray photoelectron spectroscopy. The capacity of MNC to adsorb Cr(VI) and Pb(II) was evaluated. The effects of the initial pH, dosage, concentration and temperature on the adsorption capacity of MNC were measured. MNC had a large specific surface area and a special porous structure. Its nitrogen and carbon sources were rich, and the ratio of carbon to nitrogen was fixed. The maximum Cr(VI)-adsorption capacity and maximum Pb(II) adsorption capacity of MNC could reach 456.63 and 507.13 mg·g −1 at 318 K, respectively. The pseudo-second-order model was used to describe the adsorption kinetics of MNC, and the Freundlich model was employed to discuss its isotherms. The adsorption process was affected by the electrostatic force, the reducing reaction, pores and chelation. The results of this study suggest that MNC is a material with superior performance, and is very easily regenerated, reused, and separated in the adsorption process.
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CHEMOSPHERE
·
2018
·
IF 4.427
Peng Liu,Xiangyu Wang,Jun Ma,Huiling Liu,Ping Ning
To provide superior substrates and determine the specific species of immobilized nano zero-valent iron (NZVI) system, polyacrylonitrile (PAN) membrane was functionalized by bio-inspired polydopamine (PDA) and poly( l -DOPA) (PDOPA) for efficient immobilization of NZVI. The synthesized composites were denoted as PAN/PDA-NZVI (PPN) and PAN/PDOPA-NZVI (PON), respectively. Analyses of XRD, SEM/EDS and XPS show that the aggregation and release of iron nanoparticles had been successfully controlled by improving membrane hydrophilcity and iron-chelating capacity via the graft of functionalized groups (i.e. OH and COOH) of PDA and PDOPA on PAN membrane. Both PPN and PON composites exhibited superior reactivity for Cr(VI) removal (Cr(VI) removal efficiency and reaction rate were 2.21–2.22 and 9.90–10.14 times higher than that of bare NZVI, respectively). The stability and recyclability of PPN and PON composites could be maintained over repeated cycles. Further analyses indicate that PON is more capable for Cr(VI) elimination than PPN due to the proprietary carboxyl of l -DOPA. With the addition of 1,10-phenanthroline, membrane-chelated Fe(II) was determined to be the major species in Cr(VI) removal system, accounting for 56.9% and 53.8% with regard to PPN and PON composites, and Fe 0 was responsible for the reduction of residual Cr(VI). Analyse of reacted composites revealed that Cr(VI) was completely converted into Cr(III), followed by formation of dominant Cr(III)/Fe(III) (oxy)hydroxides and partial desorption from NZVI reactive sites. This study suggested that both synthesized PPN and PON composites have potentials for Cr(VI)-contaminated wastewater treatment .
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CATALYSIS TODAY
·
2013
·
IF 2.98
Xuefeng Hu,Huanhuan Ji,Fei Chang,Yongming Luo
In this study, a rapid reduction of Cr(VI) and degradation of 2,4,6-trichlorophenol (2,4,6-TCP) in a simultaneous manner was reported through the catalysis of g-C 3 N 4 under visible light ( λ > 420 nm) irradiation. The effects of initial concentration of reactants, dissolved O 2 and pH value were investigated systematically. It indicated that, under the optimized concentration, the Cr(VI) reduction and 2,4,6-TCP oxidation could be accomplished in couple of hours in the presence of g-C 3 N 4 . And also, the O 2 involvement and low pH value were able to significantly improve the removal rate of Cr(VI) and 2,4,6-TCP. In addition, the reaction mechanism was investigated through monitoring the reduced states of Cr(VI) and active oxygen intermediates formed during photoreaction by ESR and XPS, as well as determining the degradation products of 2,4,6-TCP by HPLC–MS. The results supported that the redox reactions of Cr(VI) and 2,4,6-TCP can be performed simultaneously via a synergistic oxidation–reduction mechanism in the presence of g-C 3 N 4 under visible light irradiation.
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