Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Liudi Ji,Fei Li,Qi Jia,Yicheng Yao,Xiaoming Zhu,Zeyu Li,Peng Hu
Developing rapid and reliable electrochemical monitoring methods for 4-CP is of great significance to ensure the safety of the water environment. Electrochemical sensing materials with high sensitivity and selectivity are urgently needed. Here, interlaced sheet-like Ni-BDC frameworks (BDC: 1,4-dicarboxybenzene) and multi-walled carbon nanotubes (MWCNTs) composite (Ni-BDC/MWCNTs) are constructed via in-situ self-assembly of Ni-BDC in the presence of MWCNTs at room temperature . Because of the large specific surface area , high electrochemical activity of Ni-BDC, and the outstanding electrical conductivity of MWCNTs, the obtained Ni-BDC/MWCNTs compound had a significant signal enhancement effect for the oxidation of 4-CP based on the large electrochemical active area, fast electron transfer ability, strong accumulation ability, and high electrocatalytic rate. It was found that the electrochemical oxidation of 4-CP involved the transfer of an electron and a proton. A wide linear range (0.1–50 and 50–500 μM), low detection limit (16.5 nM), high reproducibility, strong stability, and good selectivity were achieved at the Ni-BDC/MWCNTs sensing platform. It also has been successfully used to monitor 4-CP in different river water samples, and got similar results compared to HPLC, which provides promising potential for application in water environment safety monitoring and protection.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2024
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IF 0
Sun Qing,Yu Jiale,Zhao Youpu,Liu Hanhu,Li Chunsheng,Tao Jiajun,Zhang Jian,Sheng Jiawei
Iron-based catalysts are environmentally friendly, and iron minerals are abundant in the earth's crust, with great potential advantages for PMS-based advanced oxidation process applications. However, homogeneous Fe 2+ /PMS systems suffer from side reactions and are challenging to reuse. Therefore, developing catalysts with improved stability and activity is a long-term goal for practical Fe-based catalyst applications. In this study, we prepared Fe-HNTs nanoreactors by encapsulating a nitrogen-doped carbon layer with one-dimensional halloysite nanotubes (HNTs) using the molten salt-assisted method. Subsequently, Fe (Co, Ni) nanoclusters were anchored onto the nitrogen-doped carbon layer at a relatively low temperature (550℃), resulting in stable and uniform distribution of metal nanoclusters on the surface of HNTs carriers in the form of Fe-N x coordination. The results showed that the dissolution of the molten salt and leaching of post-treated metal oxides generated numerous mesopores within the Fe-HNTs nanoreactor, leading to a specific surface area more than 10 times that of HNTs. This enhanced mass transfer capability facilitates rapid pollutant removal while exposing more active sites. Remarkably, Fe-HNTs adsorbed up to 97% of tetracycline within 60 min. In the Fe-HNTs/PMS system, the predominant reactive oxygen species has been shown to be 1 O 2 , and the added tetracycline was degraded by more than 98% within 5 min. The removal of tetracycline was maintained above 96% in the presence of interfering factors such as wide pH (3–11) and inorganic anions (5 mM Cl − , HCO 3 − , NO 3 − , and SO 4 2− ). The investigated mechanism suggests that efficient degradation and interference resistance of the Fe-HNTs/PMS system is attributed to the synergistic effect between the rapid adsorption of porous structure and the non-radical ( 1 O 2 )-dominated degradation pathway. Graphical Abstract
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CHEMICAL PHYSICS LETTERS
·
2025
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IF 3.1
Siyuan Yin,Song Li,Muying Sun,Zhongsheng Wen,Juncai Sun
Transition metal oxides (TMOs) are promising high-capacity anodes for Li-ion batteries, but their low initial Coulombic efficiency (ICE) hinders practical application. Here, a Ni/Mn 3 O 4 composite was prepared via ball milling, where nano-Ni dispersion enhanced phase transition, increasing ICE from 39.7 % to 57.8 %. Nano-Ni reduced charge transfer resistance and enhanced pseudocapacitance contribution, improving kinetics. DFT calculations revealed Ni’s catalytic role in lowering the Li O bond-breaking energy barrier and suppressing irreversible phase transitions. TEM confirmed Ni-promoted Mn 3 O 4 phase transformation and accelerated early-stage reaction kinetics. This study provides a strategy for designing conversion-type anodes with high ICE and kinetics.
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ACS Catalysis
·
2024
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IF 11.3
Xiaohong Ren,Qian Qiang,Zhuohua Sun,Ting Wei,Xiaoqiang Yu,Zeming Rong,Changzhi Li
This work demonstrates the upgrading of lignin-derived monomers through a cascade demethoxylation, aqueous-phase reforming reaction, eliminating the need for external hydrogen supply. The core of this research lies in the use of neat water as both reaction medium and the hydrogen donor over a multifunctional Ni/MgO catalyst, which is responsible for water splitting, aqueous-phase reforming of in situ generated methanol, and selective cleavage of the C–O bond, finally establishing an efficient one-pot approach achieving a high yield of phenols. Reaction mechanism studies proved that the initial H* source came from water by its splitting on the surface of the Ni/MgO catalyst, which triggered the fracture of the aromatic ether bond to afford phenols and CH3O*. The subsequent aqueous-phase reforming of CH3O* and OH* generated more hydrogen and further accelerated the hydrodeoxygenation (HDO) process. A high conversion of 87.8% with a selectivity of 88.9% for phenol could be achieved at 190 °C from guaiacol. Thanks to the interesting water-splitting mechanisms and strong metal–support interaction (SMSI), Ni/MgO exhibited significantly enhanced stability compared to the previously reported nanoporous Ni catalysts. Further, with real lignin as the substrate, 16.3 wt % combined yield of phenol and 4-methylphenol could be acquired under optimized conditions. Overall, this “H2-free” approach offers a promising alternative to conventional biorefinery processes, addressing the challenges of hydrogen sourcing and economic feasibility.
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GREEN CHEMISTRY
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2024
·Vol. 26
·期 6
·3507-3516
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IF 9.3
Xinqi Zheng,Bo Chen,Juwen Gu,Songbai Qiu,Xiaoping Wu,Qian Zhang,Tiejun Wang
Direct reconstruction of fermentation of ethanol in water with high water content to higher alcohols is a promising way to produce value-added fine chemicals and bio-fuels. In particular, aqueous ethanol reconstruction under near-ambient conditions is a milestone goal, but facing great challenges. Herein, the highly active and thermostable hexagonal-close-packed (hcp) Ni dominated hcp/fcc-Ni@C catalyst was fabricated via a facile surfactant-induced carbonization strategy for direct reconstruction of fermentation of ethanol solution to C4+ higher alcohols at near-ambient temperature (<100 °C). A superior performance of >99% higher alcohol selectivity with 17.6% ethanol conversion was achieved. DFT analysis revealed a low energy barrier of ethanol dehydrogenation (rate-determining step) over hcp-Ni, which is crucial for the ultra-low temperature ethanol reconstruction in water. The induction effect of the amide group in surfactant precursors is the key to the formation of hcp-Ni. This work provides new insight into producing bio-based higher alcohols from readily accessible aqueous fermentation of ethanol under mild reaction conditions, which is very promising for large-scale combined applications in industry.
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Nanoscale
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2025
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IF 5.1
Xi-Song Gong,Xing Liu,Jian Zhou
The development of environmentally friendly, high-efficiency, stable, earth-abundant and non-precious metal-based electrocatalysts with fast kinetics and low overpotential for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is of exceeding significance but still challenging. Herein, a bifunctional electrode of unique hierarchical NiFe-LDH/Ni/NiCo2S4/NF (NiFe-LDH = nickel–iron layered double hydroxide and NF = nickel foam) electrocatalytic architecture, which is built up from NiFe-LDH nanosheets, Ni nanoparticles and NiCo2S4 nanoneedles sequentially arrayed on a porous NF substrate, has been prepared by a facile hydrothermal and electrodeposition method. This electrocatalytic architecture is binder-free and its outer NiFe-LDH nanosheets can effectively prevent the oxidation of inner Ni nanoparticles and corrosion of NiCo2S4 nanoneedles during water electrolysis. The integration of effective HER Ni nanoparticles into OER NiFe-LDH and NiCo2S4 electrocatalysts can not only overcome the disadvantage of their poor electrical conductivity, but also greatly improve their HER and OER activities, owing to the unique hierarchical heterostructure and multicomponent synergies among Ni, NiFe-LDH, and NiCo2S4. Consequently, this electrode shows better OER performance with ultra-low overpotential of 192 mV at 10 mA cm−2, a small Tafel slope of only 37 mV dec−1 and high stability in comparison with commercial RuO2, and also exhibits excellent HER activity with a low overpotential of 83 mV at 10 mA cm−2. More importantly, the NiFe-LDH/Ni/NiCo2S4/NF composite serves as anode and cathode for overall water splitting, and it requires a low cell potential of only 1.53 V to reach a current density of 10 mA cm−2, which evidently exceeds that of the standard Pt–C/NF//RuO2/NF cell of 1.61 V. This work provides a feasible strategy to prepare high-efficiency, low-cost and non-precious metal-based electrocatalysts for overall water splitting.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Liandong Li,Ziqi Qiao,Bing Lin,Hailong Zhang,Yingying Wang,Zhe Sun,Yiping Hu,Denghao Ouyang,Shiyu Li,Hangzhou Wang,Junlei Tang,Caineng Zou
Electrolysis of neutral saline wastewater/seawater enables sustainable hydrogen production but faces sluggish hydrogen evolution reaction (HER) kinetics and poor durability in chloride-rich media. Herein, a novel Cu 2 S/Amorphous/Cu–Ni–Mo heterostructure electrocatalyst, prepared by electrodeposition and atomic layer deposition (ALD), was introduced to address these challenges. The electrode was synthesized by electrodepositing a Cu–Ni–Mo coating onto a stainless steel substrate, followed by in-situ sulfurization using ALD technology to form an amorphous layer, yielding a heterostructure with optimized interfacial properties. This heterostructure electrode exhibited an overpotential of 63.29 mV at −10 mA cm −2 and maintained stable operation at −100 mA cm −2 for over 180 h in 0.5 mol/L NaCl +1 mol/L phosphate buffered saline (PBS). A 10 cm × 10 cm electrode was successfully fabricated using this scalable method, which exhibited uniform morphology and stability exceeding 240 h. This work advances HER performance and scalability in neutral environments, facilitating industrial-scale electrocatalytic hydrogen production.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Xing Cao,Qianxi Dang,Huanhui Chen,Yubin Zhao,Ya Liu,Junrong Zeng,Qing Ma,Liubiao Zhong,Dayou Wang,Yejun Qiu
To address the severe carrier recombination in BiVO 4 -based Photoelectrochemical (PEC) water splitting, we developed Fe-doped Ni nanocrystals (Fe:Ni NCs) through an organic liquid phase synthesis as an efficient cocatalyst. Through a dip-coating and annealing modification process, the optimized Fe:Ni/BiVO 4 photoanode achieved a remarkable photocurrent density of 4.72 mA/cm 2 at 1.23 V vs. RHE, representing a 4.07-fold enhancement over pristine BiVO 4 . In-situ Raman characterization revealed that Fe:Ni NCs on BiVO 4 underwent in-situ surface reconstruction to form a unique Fe:Ni@Fe:NiOOH core–shell structure during PEC reaction. The presence of Fe accelerated the conversion of Ni to active NiOOH at lower potential (0.25 V vs. RHE) compared to pure Ni NCs modified BiVO 4 photoanode (0.30 V vs. RHE). Mechanistic studies identified a dual activation pathway involving both applied potential and BiVO 4 valence band oxidation. Meanwhile, Fe:Ni NCs cores with high conductivity accelerated the migration and accumulation of holes into Fe:NiOOH shells, resulting in improved carrier injection efficiency and water oxidation kinetics. This work not only elucidates fundamental differences between PEC and electrocatalytic water splitting mechanisms but also provides a reference for designing high-performance PEC photoanodes.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2025
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IF 4.9
Jing Li,Ying-Xia Ma,Shi-Fan Chang,Wen-Jing Li,Rui-Xiang Wu,Zhi-Da Wang,Yu-Ting Chai,Fen Ran
Metal-organic frameworks (MOFs) exhibit promising prospects as supercapacitor electrode materials due to the high specific surface area, adjustable pore structure and flexible structural design, but suffer from low conductivity, unstable structure and easy collapse. In this work, by selecting nickel (Ⅱ) nitrate hexahydrate and 2-amino-5-mercapto-1,3,4-thiadiazole (EAMTD, containing various functional groups), a series of Ni-MOFs-EAMTD samples were fabricated in a mixed solvent system of N, N-dimethylformamide and ethylene glycol. EAMTD and mixed solvents provided a coordination environment rich in S, N and O heteroatoms for Ni ions, enhancing the delocalization of charge throughout the framework. The synergistic electronic interaction improved electrical conductivity and electrochemical performance of the Ni-MOFs-EAMTD, which demonstrated a high specific capacitance of 1608.0 F·g -1 at 1 A·g -1 . And assembled into an asymmetric supercapacitor (ASC) with activated carbon, it exhibited high energy density (39.2 Wh·kg -1 ) and power density (850.0 W·kg -1 ). More significantly, the ASC exhibits self-regenerative property. After 10000 cycles, the specific capacitance of ASC dropped to 45%, then recovered to 65%, which was attributed to the decomposition of Ni-MOFs-EAMTD into smaller nanoparticles and the release of active sites to compensate for the capacitance. This work provides a feasible strategy to develop MOFs-based electrode materials, paving the way for secondary resource utilization and extended industrial chain development.
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RARE METALS
·
2025
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IF 11
Zheng Lin-Xin,Zhang Liu-Ting,Wu Fu-Ying,Li Hong,Fang Fang
Magnesium hydride (MgH 2 ) is recognized as a promising candidate for solid-state hydrogen storage due to its high hydrogen capacity and safety. However, its highly stable thermodynamics and slow kinetics pose challenges to its commercial application. To effectively solve these problems, Ni–Ti based MOFs (NT-MOF and NT-MOF- x ( x = Ar, O 2 , and H 2 )) are prepared as effective catalysts for MgH 2 , with NT-MOF-Ar/MgH 2 showing the best performance. The onset dehydrogenation temperature of NT-MOF-Ar/MgH 2 is reduced to 197 °C and remains 97% H 2 capacity after 20 cycles. An interface reconstruction which enables its superior catalytic performance is evidenced. By in situ forming a multiphase-multivalence Mg-Ni-Ti-C catalytic interface: Mg 2 Ni/Mg 2 NiH 4 act as a hydrogen pump, multivalence Ti facilitates charge transfer, while amorphous carbon mitigates agglomeration, enhancing long-term performance. Our work verifies the interface reconstruction in a MgH 2 hydrogen storage system, thus paving ways for developing new catalytic mechanisms and efficient catalysts for hydrogen storage and other energy related fields. Graphical
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Energy Storage Materials
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2025
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IF 20.2
Xingyu Hu,Hui Shi,Yilei Zheng,Penghui Shao,Liming Yang,Xubiao Luo
The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H 2 O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H 2 O) 6 ] 2+ and [CoCl 4 ] 2- in the DES-20 % H 2 O system. Furthermore, the K sp differences of the Ni-complex and Co-complex in the C 3 H 2 O 4 2- -rich environment was effectively magnified. These significant differences synergistically enable the generation of C 3 H 2 NiO 4 ·2H 2 O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Yuanhui Shen,Yunlian Liu,Ying Pan,Hongguang Jin
Chemical looping dry reforming of methane (CL-DRM) represents an innovative CO 2 utilization technology that enables efficient conversion of CH 4 and CO 2 while producing high-quality syngas. To investigate the carbon resistance of oxygen carriers, we present a comprehensive analysis of carbon deposition mechanisms in CL-DRM from both thermodynamic and experimental perspectives, establishing a quantitative correlation between carbon deposition and oxygen carrier characteristics. Experimental validation confirmed the thermodynamic predictions. Utilizing an exsolution strategy, we successfully synthesized nano-Ni-modified iron-based perovskite, which demonstrated exceptional reactivity and carbon resistance at 800 °C. This work provides both theoretical and practical guidance for the development of advanced oxygen carriers in CL-DRM systems.
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