Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xue Bai,Fengyi Sun,Liyan Ma,Zhuwu Jiang,Hongcheng Di,Chuntao Pan,Fengying Zhang,Jiahan Yang,Hongyu Zhang
A green and sustainable three-dimensional particle electrodes system with nickel-iron layered double hydroxide mixing activated carbon particles (NiFe-LDH/AC) as particle electrodes is used in this work. Its employment in degradation of N-Nitrosodiethylamine (NDEA), A type of nitrosamines disinfection byproducts (NAs) widely present in water bodies, exhibiting significant degradation efficiency at close to neutral pH. Response surface methodology (RSM) is used to analyze the interaction effects and predict optimal conditions of four operating parameters (influent water flow, electrolyte concentration, current density and initial concentration) on the NDEA degradation efficiency. Calculated coefficients of determination (R 2 ) are higher than 0.997 for all responses according to analysis of variance. At optimum conditions, a maximum degradation efficiency of 71.88% is achieved for NDEA. The results of electron paramagnetic resonance (EPR) and free radical quenching experiments indicate that the degradation of NDEA in the 3D AER system is dominated by •OH. Furthermore, based on the recognition of main reaction intermediates by GC-MS and density functional theory (DFT), possible degradation pathway is proposed and toxicological evaluation of degradation products is made. Our research provides a promising alternative method for the efficient and environmentally friendly removal of NAs from water.
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ACS Sustainable Chemistry & Engineering
·
2025
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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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CHEMICAL ENGINEERING JOURNAL
·
2025
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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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MATERIALS RESEARCH BULLETIN
·
2025
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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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ACS Applied Materials & Interfaces
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2021
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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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ChemCatChem
·
2026
·Vol. 18
·期 5
·e01665
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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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CRYSTENGCOMM
·
2020
·Vol. 23
·期 5
·1172-1180
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IF 3.117
Qibing Dong,Chao Shuai,Zunli Mo,Ruibin Guo,Nijuan Liu,Guigui Liu,Jia Wang,Wentong Liu,Ying Chen,Jingjing Liu,Yangyang Jiang,Qinqin Gao
A Ni-based metal organic framework (Ni-BDC) and subsequently derived NiFe-LDH were studied to overcome the defect of the low availability of active sites for the oxygen evolution reaction (OER) during the water splitting process. This work reported NiFe-LDH nanosheets with an ultra-thin structure through an in situ surface-conversion derived from Ni-BDC. The unique structure and characteristic morphology were confirmed using X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy, and the OER activities of the catalysts were systematically studied. The obtained results indicated that the synthesized Ni-BDC@NiFe-LDH-2 showed excellent OER activity, with a low overpotential of 272 mV at a current density of 10 mA cm−2, a small Tafel slope of 45 mV dec−1, and excellent stability, owing to the addition of abundant metal sites and the expansion of the electron transport channels during the conversion process to form the ultra-thin layer structure. This work provides a novel strategy for the application, design, and manufacture of metal organic framework (MOF)-based high-efficiency active materials.
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Advanced Energy Materials
·
2024
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IF 24.4
Yanyan Zhang,Guangtong Hai,Zhuoshen Huang,Zhimeng Liu,Xiubing Huang,Ge Wang
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR) is an effective route to produce value-added chemicals with low energy consumption. In this work, efficient electrocatalysts are prepared by varying the amount of Ce doping and CeO 2 modification on NiFe layered double hydroxide (NiFe–LDH) nanosheets supported on carbon cloth (CC). Through Ce doping and heterogeneous interface construction, the electronic structure and coordination chemistry of NiFe–LDH are greatly changed. Compared to CeO 2 modification and the synergistic effect of Ce-doping and CeO 2 modification, CC@NiFeCe(3%)-LDH with only Ce-doping show excellent charge transfer ability, higher HMF conversion (95.73%), 2,5-furandicarboxylic acid (FDCA) selectivity (93.31%), and Faraday efficiency (99.47%) at only 1.44 V RHE . Density-functional theory calculations and X-ray fine structure spectroscopy demonstrate that Ce doping, compared with CeO 2 modification and their synergistic effects, significantly facilitates the electron transport and optimizes intermediate adsorption by effectively lowering the activation energy for the transformation of 5-formyl-2-furancarboxylic acid (FFCA) and encourage the conversion of FFCA to FDCA. Overall, this work systemically investigates the HMFOR behaviors of CC@NiFe–LDH under Ce doping, CeO 2 modification, and their synergetic effect, which provides some guidance on the development of high-performance electrocatalysts for HMFOR performance.
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Small
·
2024
·
IF 13
Huan Xu,Xiao Sun,Lingtong Ding,Jingjing Liu,Dan Zhang,Minmin Liu,Xiao Wang,Qixian Zhang,Jiujun Zhang
Electrochemical water-electrolysis for hydrogen generation often requires more energy due to the sluggish oxygen evolution reaction (OER). This work introduces a double-layered nanoflower catalyst, NiFe-LDH@S-NiFeO x /NF, featuring a crystalline NiFe-LDH coating on amorphous S-NiFeO x on nickel foam. Strategically integrating a crystalline-amorphous (c-a) heterostructure leverages strain engineering to enhance OER activity with low overpotentials ( η 100 = 220 and η 500 = 245 mV) and stability (135 h at η 100 and 80 h at η 500 ). Theoretical density functional theory (DFT) calculations reveal that the compressive strain can optimize the adsorption of oxygen-containing intermediates to reduce the reaction energy barrier, thus improving the reaction kinetics and performance of OER. Moreover, its phosphated derivative, NiFeP@S-NiFeO x /NF, exhibits high hydrogen evolution reaction (HER) performance ( η 10 = 64 mV, η 100 = 187 mV). An alkaline water-electrolysis cell of NiFeP@S-NiFeO x /NF(−)||NiFe-LDH@S-NiFeO x /NF(+) requires only a cell voltage of 1.77 V at 100 mA cm −2 , demonstrating excellent stability over 110 h (at both 10 and 100 mA cm −2 ). This work highlights the benefits of integrating crystal-amorphous interfaces and strain effects, offering insights into the understanding and optimizing catalytic OER mechanism and advancing water-electrolysis technology.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Ayaz Muzammil,Rizwan Haider,Wenrui Wei,Lin Li,Liang Wu,Yi Fan,Xianxia Yuan
The development of highly efficient oxygen evolution reaction (OER) electrocatalysts is pivotal to enhance the performance of alkaline water electrolyzers. Herein, a facile two-step electrodeposition method is developed for the fabrication of nitrogen-doped carbon (NC) and manganese-incorporated NiFe layered double hydroxides (LDHs) supported on Ni foam (NF). When evaluated in 1.0 M KOH solution, the optimized material of NC20-Mn-NiFe LDH showed excellent OER performance requiring low overpotentials of 298 and 331 mV to achieve high current densities of 500 and 1000 mA cm–2, respectively, and no loss in current density was observed at fixed potentials of 1.53 and 1.57 V for 125 h in each case. This performance is not only better than that of the state-of-the-art RuO2/NF but also most of the recently reported LDH-based catalysts. Such a remarkable performance is mainly attributed to the vertical growth of NC20-Mn-NiFe LDH sheets on NF, facilitated electron transfer and charge density modulation on the active metal sites due to the electron-withdrawing and electron-donating effects of NC and Mn, respectively, resulting in the shift of the rate-determining step from OOH* formation to O2 desorption with decreased free energy. This research work provides further insights into modulating the structure of LDH-based materials to achieve a high OER performance delivering industrial-level current densities at low overpotentials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Longlong Liu,Zunpeng Hu,Minghui Wang,Jinliang Ma,Zihao Chen,Xin Ning,Ding Yuan
The construction of a hybrid hierarchical architecture is a promising strategy for optimizing the electrocatalytic activity and the performance of flexible Zn-air battery. However, it still remains a challenging task. This study reports on the use of a simple approach in the preparation of a flexible 3D self-supporting bifunctional catalyst. Ultrathin NiFe-based layered double hydroxide nanosheets (NiFe-LDH) have in this approach been strongly coupled to a metal-organic framework (MOF)-derived carbon nanoflake array, to be used in flexible Zn-air batteries. Importantly, the introduction of Co nanoparticles that were anchored onto the nitrogen-doped porous carbon (Co-NC) nanoflakes provided an abundance of active sites for the oxygen reduction reaction (ORR). Moreover, the catalytic oxygen evolution reaction (OER) process was improved by altering the local electronic structure of the Ni and Fe species in NiFe-LDH. The 3D interconnected conductive network structure, in addition to the strong coupling between NiFe-LDH and Co-NC, was found to give a catalyst with superior electrocatalytic OER performances. The overpotential was only 284 mV at 50 mA cm −2 in an alkaline medium, which is a result that outperforms the commercial RuO 2 catalyst. This bifunctional catalyst did also exhibit a good catalytic performance that is comparable to that of commercial Pt/C towards ORR. Interestingly, when this catalyst was used as binder-free air cathode, the assembled flexible solid-state Zn-air battery demonstrated a favorable power density, cycling stability, and mechanical flexibility. The present work offers a facile and efficient strategy for the development and construction of self-supporting bifunctional OER/ORR electrocatalysts , to be used in wearable and flexible electronic devices.
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