Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zhuo Zeng,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Jiangfu Zheng
In advanced oxidation processes (AOPs) based on peroxynitrite (PMS), generating reactive radicals efficiently and consistently is challenging due to high electron occupancy and slow conversion rates of PMS. In this study, ultrathin In 2 O 3 with oxygen vacancies (Ov) was combined with ultrathin ZnAl-LDH to construct S-scheme In 2 O 3 -Ov/ZnAl-LDH-Ov heterojunctions. The presence of Ov promotes the formation of charge-transfer channels (Al-O-In bonding) at the interface of these heterojunctions, thereby reducing electron occupancy and enhancing the generation of active radicals in the InLDH/PMS/Vis system. This S-scheme heterojunction facilitates the acceleration of photogenerated electrons, leading to the rapid conversion of PMS into hydroxyl (•OH) and sulfate radicals (SO 4 - •), and promotes swift electron transfer. Consequently, the InLDH/PMS/Vis system demonstrates exceptional degradation efficiency for a wide range of organic pollutants and a high removal capacity in treating real industrial wastewater. This investigation offers a novel perspective on the coordination mechanisms between photocatalysis and PMS activation.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuanmeng Lou,Zhaotian Ba,Zhaodi Yuan,Jian Li,Cui Li,Lili Ma,Xiujuan Wang,Xin Wen,Pingan Song
The development of carbon fiber reinforced epoxy resin (EP/CF) composites with good balance on flame retardancy and mechanical properties remains a critical challenge. Inspired by the rod@sheets hierarchical structure of corncobs, herein a novel CF/PO 4 3− intercalated NiFe-LDH hybrid (CF@NiFe-LDH-P) was successfully fabricated via in-situ growth of NiFe-LDH nanosheets on CF surfaces, followed by PO 4 3− intercalation via an ion-exchange process. Subsequently, the as-synthesized CF@NiFe-LDH-P was incorporated with EP matrix. The resultant EP/CF@NiFe-LDH-P composites exhibited remarkable improvements in flame retardancy, including the limiting oxygen index (LOI) value of 36.8 %, UL-94 V0 rating, and a 66.8 % reduction in the peak of heat release rate (PHRR). According to the structure/composition analysis of residual char, the flame-retardant mechanism was mainly ascribed to the synergistic effect between NiFe-LDH and PO 4 3− , where NiFe-LDH catalyzed the carbonization of EP fragments into graphitized carbon, while PO 4 3− enhanced the cross-linking of char network through phosphate ester bonds. Meanwhile, the flame retarded EP/CF@NiFe-LDH-P composites displayed superior mechanical performances. Compared to the pristine EP/CF, EP/CF@NiFe-LDH-P displayed outstanding mechanical properties in Young's modulus (+26.9 %), tensile strength (+26.2 %) and impact strength (+39.4 %). These enhancements were attributed to the corncob-like structure of CF@NiFe-LDH-P, which established strong interfacial adhesion with EP via hydrogen bonding. This work presents an innovative bio-inspired strategy to achieve synergistic optimization of flame retardancy and mechanical performances in EP/CF composites, paving the way for their expanded applications in high-performance engineering and advanced technological fields.
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高影响因子
LANGMUIR
·
2024
·
IF 3.7
Fei Zhu,Yingqing Zhan,Ximin Chen,Yiwen Chen,Yajie Lei,Hongshan Jia,Yinlong Li,Xinyue Duan
The synergistic treatment of oily wastewater containing organic hazards and emulsified oils remains a big challenge for membrane separation technology. Herein, the photocatalytic membrane, which combined the physical barrier and catalytic oxidation-driven degradation functionality, was fabricated via anchoring a nanoflower-branched CoAl-LDH@PANI Z-scheme heterojunction onto a porous polyacrylonitrile mat and using tannic acid as an adhesive. The assembly of such a Z-scheme heterojunction offered the superior photocatalytic degradation performance of soluble dyes and tetracycline (up to 94.3%) to the membrane with the improved photocatalytic activity of 2.33 times compared with the CoAl-LDH@pPAN membrane. Quenching experiments suggested that the •O2– was the most reactive oxygen species in the catalytic reaction system of the composite membrane. The greatly enhanced photocatalytic activity was attributed to the effective inhibition of photogenerated hole–electron combination using PANI as a carrier, with charge transferring from LDH to PANI. The possible photocatalytic degradation mechanism was proposed based on VB-XPS, electron spin resonance spectroscopy, and DRS technologies, which was confirmed by density functional theory calculation. Meanwhile, benefiting from the superhydrophilic/oleophobic feature and low oil adhesion, the membrane exhibited high permeability for isooctane emulsion (3990.39 L·m–2·h–1), high structure stability, and satisfactory cycling performance. This work provided a strategy to develop superwetting and photocatalytic composite membranes for treating complex multicomponent pollutants in the chemical industry.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chi Zhang,Zhixiao Zhu,Yanke Zhang,Weixuan Shao,Di Wu,Guannan Peng,Zhengchun Liu
In-plane micro-supercapacitors (IMSCs) have greater promise for use in flexible wearable electronics than traditional stacked configurations due to their ease of integration and conformability. Nickel-cobalt layered double hydroxide (NiCo-LDH) has garnered significant interest as a stellar material for supercapacitors because of its affordable price, regular morphology, and high theoretical capacity. Unfortunately, the intrinsic poor conductivity of LDH materials prevents supercapacitors from achieving long-term stable cycling and the desired energy density. This research successfully applies the self-templated approach to prepare carbon nanotubes (CNTs) with heterogeneous architectures and numerous phase interfaces, thereby mitigating this disadvantage. Carbon nanosheets adorned with WO 2 and MoO 2 nanoparticles assemble the CNT with a typical three-dimensional structure. When combined with LDH in a suitable ratio, the composite electrode’s conductivity significantly improves, providing increased capacity and cycling stability. Compared to commercial CNTs , the larger size of the prepared WO 2 /MoO 2 @P, N-CNTs serves a superior supporting and connecting role, thereby preventing the NiCo-LDH from aggregating. Under the best conditions, the composite electrode demonstrates a capacity of 1237 C/g at 1 A g −1 and an optimal capacity retention of more than 92%. For the IMSC devices, the composite materials as the positive electrode achieve an energy density of 0.0590 mWh cm −2 , and no capacity degradation is observed after 10,000 cycles. In addition, bending tests have demonstrated the mechanical stability of the IMSCs. Therefore, this strategy of mixing highly conductive WO 2 /MoO 2 @P, N-CNTs can effectively improve the conductivity of the composite material and the mechanical properties of the overall device. Furthermore, this concept can be further extended to the preparation and application of other wearable devices.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Dongxu Zhang,Weixuan Dong,Yanhong Liu,Xiaoqing Gu,Tianyu Yang,Qiang Hong,Di Li,Dongqi Zhang,Hongbo Zhou,Hui Huang,Baodong Mao,Zhenhui Kang,Weidong Shi
Photoassisted electrocatalysis (P-EC) emerges as a rising star for hydrogen production by embedding photoactive species in electrocatalysts, for which the interfacial structure design and charge transfer kinetics of the multifunctional catalysts remain a great challenge. Herein, Zn-AgIn5S8 quantum dots (ZAIS QDs) were embedded into 2D NiFe layered double hydroxide nanosheets through a simple hydrothermal treatment to form 0D/2D composite catalysts for P-EC. With evidence from transient photovoltage spectroscopy, we acquired a clear and fundamental understanding on the kinetics of charge extraction time and extraction amount in the 0D/2D heterojunctions that was proved to play a key role in P-EC. Upon light illumination, for HER, the optimized NiFe-ZAIS exhibits obviously reduced overpotentials of 129 and 242 mV at current densities of 10 and 50 mA cm–2, which are 22 and 33 mV lower than those of dark electrocatalysis, respectively. For OER, the NiFe-ZAIS electrode also shows low overpotentials of 220 and 268 mV at current densities of 10 and 50 mA cm–2, respectively, under light illumination, which were able to almost double the intrinsic activity. Finally, with NF@NiFe-ZAIS as both the cathode and the anode, the assembled electrolyzer only requires 1.62 V to reach the overall water splitting current density of 10 mA cm–2 under P-EC. This work provides a useful example for the profound understanding of the design and the kinetics study of multifunctional P-EC catalysts.
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Carbon Neutralization
·
2025
·Vol. 4
·期 6
·e70069
·
IF 12
Lisha Liu,Mingyuan Gao,Mengwei Guo,Rongrong Deng,Cunying Xu,Yan Li,Juanjian Ru,Yixin Hua,Qibo Zhang
The development of layered double hydroxides (LDHs) has been hindered by the mismatch between their rate capability and areal capacity at ultrahigh mass loadings. Herein, we address this issue by designing NiCo-LDH/NiCoOOH composite films with an open-pore nanosheet structure. These films are fabricated using a ChCl-urea based deep eutectic solvent (DES) additive-assisted electrodeposition method followed by electrochemical activation, and confined on each graphene nanolayer of a 2D hierarchical expanded graphene paper (EGP) substrate. This design facilitates rapid charge transport and ion diffusion, enhancing active material utilization. The DES additive induces lower crystallinity and more disordered lattices with vacancies in the composite films, strengthening the synergistic effect with the EGP interface. Consequently, the films achieve high areal capacities of 3.4 mAh cm −2 at 23 mg cm −2 mass loading (84.1% rate capability) and a record 16.6 mAh cm −2 at ultrahigh 100 mg cm −2 mass loading (58.4% rate capability, GP thickness 0.15 mm). We also elucidate the relationship between GP substrate thickness and electrochemical performance. The resulting asymmetric supercapacitor delivers an ultrahigh energy density of 6.4 mWh cm −2 and power density of 64 mW cm −2 . This study provides new insights into constructing high-mass-loading energy storage materials through microstructure regulation and interface engineering for practical applications.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
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IF 7.963
Cheng Ye,Jing Deng,Lingyi Huai,Anhong Cai,Xiao Ling,Hongguang Guo,Qiongfang Wang,Xueyan Li
Organoarsenic contaminants existing in water body threat human health and ecological environment due to insufficient bifunctional treatment technologies for organoarsenic degradation and inorganic arsenic immobilization. In order to safely and efficiently treat organoarsenic contaminants discharged into the aquatic environment, Co-Mn-Fe layered double hydroxide (CoMnFe-LDH) and Co-Mn-Fe layered double oxide (CoMnFe-LDO) were fabricated and employed as peroxymonosulfate (PMS) activator for organoarsenic degradation and inorganic arsenic immobilization, and p -arsanilic acid ( p -ASA) was selected as target pollutant. Results demonstrated that the satisfactory removal of p -ASA (100.0%) in both CoMnFe-LDH/PMS and CoMnFe-LDO/PMS systems was obtained within 30 min, and substantial inorganic arsenic adsorption could be achieved (below 0.5 mg/L) in two systems with converting major inorganic arsenic species to arsenate. As XPS, ESR and quenching experiment revealed, the existence and generation of surface-bound radicals in two systems were identified. Based on density functional theory calculation and XPS analysis, the catalytic mechanism of CoMnFe-LDO/PMS system that PMS could be activated via direct electron transfer from adsorbed p -ASA was clarified, which differed from PMS activation via coupling with surface hydroxyl groups in CoMnFe-LDH/PMS system. Catalytic performance assessment under various critical operation parameters indicated that CoMnFe-LDH presented more stable ability of p -ASA removal in a wide pH range and complex aquatic environment. The recycle experiment demonstrated the excellent stability and reusability of CoMnFe-LDH(LDO). Besides, seven degradation products of p -ASA in CoMnFe-LDH/PMS system including phenolic compounds , azophenylarsonic acid, nitrobenzene and benzoquinne were identified by UV–Vis spectra and LC-TOF-MS analysis, and the corresponding degradation pathway was proposed. In summary, compared to CoMnFe-LDO/PMS, CoMnFe-LDH/PMS holds great promise for the development of an oxidation-adsorption process for efficient control of organoarsenic pollutant.
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MATERIALS RESEARCH BULLETIN
·
2025
·
IF 5.7
Xiaoguang San,Xueying Li,Wanmeng Wu,Lei Zhang,Jian Qi,Ming Wang,Dan Meng
In oxygen evolution reaction (OER) electrocatalysis, conventional NiFe-LDH suffers from poor performance due to interlayer stacking (masking active sites) and low intrinsic conductivity (charge transfer hysteresis). In order to overcome this bottleneck, a series of NiFe-LDH/MOF heterojunction electrocatalysts with self-supported hierarchical structures and varying iron contents were in-situ constructed on nickel foam via a simple hydrothermal method using an in-situ "self-dissociation-assembly" strategy. Among them, Ni 0.66 Fe 0.33 -LDH/MOF excelled, showing an overpotential as low as 232 mV at 50 mA cm -2 , surpassing some noble metal catalysts. Electrochemical tests and characterization results revealed that the performance enhancement originates from the heterojunction structure: Firstly, the interfacial coupling between the MOF and LDH provides efficient electron transport pathways. Secondly, the heterojunction induces the formation of oxygen vacancies and optimizes the electronic structure of the metal centers, thereby improving the reaction kinetics. This work provides new insights for designing high-performance non-precious metal OER electrocatalysts.
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高影响因子
CELLULOSE
·
2024
·Vol. 31
·期 6
·3517-3531
·
IF 4.9
Zhang Shanbei,Chen Zanmei,He Hongwei,Jiang Yijun
The alkali/urea system is an economical and environmentally friendly solvent system for dissolving cellulose. However, the mechanical performance of cellulose derived materials (such as fibres or films) treated with alkali/urea must be improved. The capacity of this system for cellulose dissolution is limited and the mechanical properties of the regenerated cellulose fibres are still unsatisfactory. Here, cotton linter pretreated with peracetic acid (PAA) was dissolved in a LiOH/urea aqueous suspension in which Zn–Al layered double hydroxide (Zn–Al LDH) nanosheets (NS thickness = 3 nm) were exfoliated in situ. After wet spinning, the strength and toughness of the regenerated cellulose fibres reached 290 ± 7.66 MPa and 23.5 ± 4.40 MJ/m 3 respectively, which were 66.7% and 150% higher than those without the LDH NS treatment. It is interesting to note that the synergistic effect of Zn 2+ and Al 3+ distributed on the surface of the LDH host layer significantly improved the solubility of cellulose at low temperature and the interaction between the cellulose and LDH NSs also improved the mechanical performance. This work provides a strategy for improving both the solubility of cellulose in the alkali/urea system and the mechanical properties of regenerated cellulose fibres. Graphical abstract
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Jinlong Zhang,Yuxiang Jin,Zhiqiang Xu,Yizhi Du,Yawen Xu,Xiaoli Ren,Bing Xue,Daoxin Liu,Yongfu Zhu,Fangfei Li
Modulating the electronic state of nickel is a crucial strategy for activating lattice oxygen participation in the oxygen evolution reaction (OER). Herein, a sol–gel-assisted hydrothermal strategy is employed to synthesize sulfate-intercalated NiFe-LDH (SG-S-NiFe-LDH), where SO42– anions are stably incorporated into the interlayer galleries to modulate Ni oxidation states. This interfacial regulation reconstructs the local electronic environment, enabling the formation of high-valent Ni species and favoring a lattice-oxygen-mediated (LOM) pathway. Structural characterizations confirm successful anion incorporation, while post-OER XPS evidences Ni3+/Ni4+ enrichment. Mechanistic studies, including pH-dependent kinetics and O–O intermediate trapping, further validate LOM dominance. SG-S-NiFe-LDH exhibits outstanding activity with a low overpotential of 177 mV at 10 mA cm–2, a Tafel slope of 32.98 mV dec–1, and long-term durability exceeding 170 h. Post-OER HRTEM and ICP confirm structural robustness and minimal Ni loss. Density functional theory calculations reveal that sulfate intercalation raises the Ni d-band center, strengthens *OOH adsorption, and reduces the *OOH → *OO barrier to 0.53 eV. Moreover, a water-splitting device using SG-S-NiFe-LDH as the anode achieves 100 mA cm–2 at 1.66 V with stable 28 h operation. Faradaic efficiency above 98% with an O2:H2 ratio of 1:2 confirms high reaction selectivity. This work demonstrates a targeted anion intercalation strategy to modulate transition-metal states, unlock lattice oxygen reactivity, and advance efficient and durable water electrolysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Tingying Zhou,Hongqiang Wang,Shunqing Feng,Eming Hu,Yonggen Deng,Yucheng Su,Jiaang Tian,Qingliang Wang
Phosphate precursor chemistry regulates FeAl-LDH structure and U(VI) capture. • H2PO4−-derived FeAl-LDH balances site accessibility and reversibility. • U(VI) removal is dominated by inner-sphere coordination with O-donor sites. • Electrostatic enrichment and open galleries provide auxiliary enhancement. • Precursor regulation offers an alternative to conventional post-modification. Understanding how phosphate precursor chemistry regulates the structure and U(VI) capture performance of layered double hydroxides (LDHs) remains challenging, as most studies focus on phosphorus loading rather than precursor-dependent phosphate chemistry. In this work, FeAl-LDH materials were synthesized using H 2 PO 4 − , HPO 4 2− , and PO 4 3− as phosphate precursors under identical conditions to investigate their effects on interlayer structure and U(VI) adsorption. Among the three precursor systems, the H 2 PO 4 − -derived material showed the most favorable balance of pore accessibility, phosphorus‑oxygen site availability, and adsorption-desorption reversibility. ICP-OES results further showed that higher phosphorus incorporation did not correspond to higher U(VI) uptake, indicating that adsorption performance depends more strongly on the chemical environment and accessibility of phosphate-derived sites than on phosphorus loading alone. The optimized FeAl-LDH-P(0.3) exhibited a Langmuir-fitted theoretical maximum adsorption capacity ( q ₘ) of 1117.21 mg/g and achieved 98% U(VI) removal from uranium-tailings pore water and leachate. Mechanistic analyses indicate that U(VI) removal is dominated by inner-sphere complexation with Fe/Al-OH and phosphorus‑oxygen sites, while electrostatic pre-enrichment and enhanced mass transfer through accessible interlayer/pore channels act as auxiliary effects. These results demonstrate that phosphate precursor chemistry can regulate the final phosphate-containing environment and structure-performance relationship of FeAl-LDH for selective uranium capture. Download: Download high-res image (339KB) Download: Download full-size image
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高影响因子
ChemCatChem
·
2026
·Vol. 18
·期 5
·e01665
·
IF 4.1
Weimi Ding,Guoshuai Fu,Ruiqi Xu,Yifan Li,Guowei Yang,Shuang Li,Pu Liu
Developing efficient and durable oxygen evolution reaction (OER) electrocatalysts is essential for scalable hydrogen production via water splitting. While NiFe-layered double hydroxides (LDHs) are promising low-cost catalysts, their catalytic performance and stability remain limited. In this study, we report a one-step laser ablation in liquid (LAL) strategy to synthesize low-loading Ru-doped NiFe-LDH nanosheets (NiFeRu/C-LDH) with precisely controlled electronic and structural properties. The laser-driven uniform incorporation of Ru 4 + into the NiFe-LDH lattice induces contraction and optimization of the local coordination environment. The resulting catalyst achieves low overpotentials of 236 and 299 mV at 10 and 100 mA cm − 2 , respectively, in 1 M KOH, outperforming commercial IrO 2 and undoped NiFe/C-LDH. It also demonstrates high durability with 95.3% activity retention after 200 h of continuous operation. Combined experimental and Density functional theory (DFT) calculations, the theoretical analyses reveal that strong Ru–O coordination and enhanced electronic interactions activate adjacent Fe sites, and establish a Fe–Ru dual active center configuration that facilitates OH − adsorption and lowers the energy barrier of the rate-determining O–O coupling step. This work offers a scalable laser-based synthesis route for high-performance electrocatalysts with tailored active sites.
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高影响因子
危险品化学品经营许可证（带存储）