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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS · 2021 · IF 2.993

Self-assembly of 1D FeSe2 chains and Fe(dien)2 complexes for ferrimagnetic inorganic-organic hybrid cuboids

Desheng Pan,Qifeng Kuang,Peng Tong,Wei Tong,Liubing Fan,Jing Zhao,Da Li,Chuljin Choi,Zhidong Zhang

Challenges still remain in producing room-temperature ferromagnetism/ferrimagnetism in inorganic–organic hybrid compounds. Here, we report the Fe vacancy-doped inorganic–organic (Fe x Se 2 ) 2 Fe(dien) 2 (dien = diethylenetriamine, x  = 0.86) hybrid cuboids by self-assemble of finite one-dimensional (1D) FeSe 2 chains and Fe(dien) 2 complexes. A growth model is proposed by kinetically controllable syntheses of novel Fe 2x+1 Se 4 (dien) 2 hybrids. The Rietveld refinement reveals that Fe vacancies in the Fe 2.71 Se 4 (dien) 2 hybrid cuboids induce large distortions of the FeSe 2 chains and the room-temperature lattice parameters are a = 9.225(4) Å, b = 18.021(8) Å and c = 11.609(6) Å. Magnetic measurements and electron spin resonance spectra of the Fe 2.71 Se 4 (dien) 2 hybrid cuboids show the ferrimagnetism with the Curie temperature (T C ) of 600 K and the spin glass state with the freezing temperature (T f ) of 108 K. Impressive room-temperature ferrimagnetic properties of the Fe 2.71 Se 4 (dien) 2 hybrid cuboids were ascribed to the high concentration of Fe 3+ vacancies (0.29 per cell) in the hybrid cuboids, which is supported by the 57 Fe Mössbauer spectrum fitting based on the ferrimagnetic model.

研究领域: 材料科学 · 磁学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Activating active motifs in Ni-Fe oxide by introducing dual-defect for oxygen evolution reaction in alkaline seawater

Yucheng Wu,Yanli Yu,Wei Shen,Yimin Jiang,Rongxing He,Ming Li

Developing simple and energy-saving pathways to prepare high-efficient and robust non-noble metal based electrocatalysts remains a huge challenge to hydrogen production from seawater electrolysis. Here we demonstrate a facile hydrothermal-calcination-etching approach that simultaneously achieves the required surface N doping and Fe vacancies generation to activate the Ni-O-Fe active motifs in N -v Fe -NiFe 2 O 4 /NF. The unique localized environments (Ni- N -Fe structures and unsaturated O- and N -coordination) due to dual-defect strategy can effectively regulate the electronic structure of the Ni-O-Fe motif to make the motif more reactive. As a result, the N -v Fe -NiFe 2 O 4 /NF catalyst exhibits overpotentials of 210, 213 and 222 mV to deliver 100 mA cm −2 in 1.0 M KOH, simulated seawater and alkaline seawater environments, respectively. Theoretical calculations prove that the Ni-O-Fe structure is the active motif and that the presence of special localized environments can optimize the adsorption of key intermediates on the activated active motifs.

CAS / MDL: 7782-61-8 57-13-6
研究领域: 材料科学 · 电化学 · 可再生能源
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts

Yiyue Zhai,Xiangrong Ren,Yu Sun,Deng Li,Bolun Wang,Shengzhong (Frank) Liu

The role of multiple vacancies containing cation and anion defects in NiFe layered double hydroxide (LDH) is still worth pursuing in electrocatalytic oxygen evolution reaction (OER). Herein, a strategy integrating the oxygen and iron vacancies is proposed to fabricate NiFe LDH with highly efficient OER performance. More Fe vacancies have been introduced with increasing Fe content in NiFe-LDH structure; operando electrochemical characterizations and density functional theory (DFT) calculations reveal that the synergic effect between the iron and the oxygen vacancies promotes the generation of reconstructed active layers, optimizing the adsorption free energy of oxygen-containing intermediates. More importantly, active NiOOH intermediate species induced by oxygen vacancies are associated with OH - intercalation pseudocapacitance, activating lattice oxygen during water oxidation . The as-prepared Ni 0.3 Fe 0.7 -LDH@NF showed ultralow overpotentials of 184 and 287 mV to achieve 10 and 400 mA·cm -2 , respectively. Our work provides a new paradigm for designing high-efficiency OER electrocatalysts.

CAS / MDL: 12125-01-8 12030-49-8
研究领域: 材料科学 · 电化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Structural reinforcement and nucleation regulation via Fe vacancy engineering for high-performance regenerated LiFePO4 cathodes

Yi Fan,Jirui Song,Yongyou Su,Yun Luo,Le Tian,Qingfeng Liu,Zitong Fei,Chenchen Li,Qi Meng,Peng Dong,Yingjie Zhang

The widespread utilization of LiFePO 4 (LFP) batteries has rendered the green regeneration of spent LFP cathode materials (SLFP) an urgent priority. Selective lithium extraction strategies have rapidly advanced through enabling simplified yet efficient lithium recycling. However, under acidic conditions, minor Fe dissolution was observed to significantly reduce the structural stability of regenerated LFP materials while exacerbating Li/Fe antisite defects. A novel strategy based on Fe vacancy site-mediated bond energy reinforcement and nucleation regulation was proposed to achieve structural reinforcement and high-efficiency regeneration. Experimental characterization revealed that Li/Fe antisite defects in regenerated materials were reduced from 1.48 % to 0.93 %, with grain size being significantly refined. The regenerated material exhibited a reversible capacity of 150.2 mAh·g −1 at 1C rate, maintaining 94.74 % capacity retention after 500 cycles, while its discharge capacity at 5C rate was elevated by 60 mAh·g −1 . Environmental and economic assessments conducted via the everbatt model demonstrated significant advantages of this strategy.

研究领域: 材料科学 · 电化学 · 储能技术 · 环境科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Atomic cation-vacancy modulated peroxymonosulfate nonradical oxidation of sulfamethoxazole via high-valent iron-oxo species

Xiaoyue Zhou,Renli Yin,Jieqiong Kang,Zhenjie Li,Yanan Pan,Jieyun Bai,Adela Jing Li,Rongliang Qiu

The formation of high-valent active species during peroxymonosulfate (PMS) activation has attracted great interest. However, how to rapidly generate high-valent active species during PMS activation process remains ambiguous. Herein, iron vacancy anchored layered double hydroxides activated PMS process were designed to enhance the removal rate of sulfamethoxazole (SMX) by 30.0 times to PMS alone, which even showed much superiority to the homogeneous Fe 2+ /PMS system. Due to the cooperation of Fe vacancies, PMS favored to be adsorbed on Fe2 sites (adjacent to iron vacancy) and combined with Fe2 sites to form Fe(II)-O-SO 3 -OH complex. Then, the accepted electrons led to the cleavage of S-O bond in Fe(II)-O-SO 3 -OH complex, resulting in the spontaneous generation of Fe (IV) =O/Fe (V) =O species. Finally, PMS activation pathways were proposed from radical oxidation to nonradical oxidation via high-valent iron-oxo species. This study provides a new perspective on generation of high-valent iron-oxo species for excellent performance and resistance with real wastewater .

研究领域: 环境化学 · 水处理 · 高级氧化工艺
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Materials Today Chemistry · 2025 · IF 6.7

Harvesting prominent room-temperature layered organic ferrimagnetic semiconductors: the importance of interfacial coordination

Xiaoling Men,Fei Qin,Xiaolei Shang,Ruiqi Huang,Jingzhen Zhou,Qifeng Kuang,Desheng Pan,Teng Yang,Jianqi Huang,Da Li,Baojuan Dong,Gang Liu,Zhidong Zhang

The emergence of ferromagnetism inherent to two-dimensional (2D) layered organic-inorganic semiconductors is challenging due to weak magnetic interactions at organic/inorganic interfaces. Here, layered room-temperature ferrimagnetic n-type semiconductor single crystalline nanosheets were synthesized by assembling iron vacancy doped β -Fe 3 Se 4 host layers and organic Fe(peha) (peha = pentaethylenehexamine) spacer layers. Structural optimization calculations reveal a bi-stable structure of ( β -Fe 2.75 Se 4 ) 4 [Fe(peha)], where Fe 2+ (peha) complexes can transit from coordinating with top of Fe vacancies (A-type) to apical Se atoms (B-type) of β -Fe 2.75 Se 4 host layers at higher energy levels. The as-synthetic nanosheets exhibit a magnetization under 50 kOe ( M 50 ) of 0.14 μ B /f.u. and a coercivity ( H C ) of 0.82 kOe at 300 K. Upon heating to 450 K, the structural transition from A-type to B-type coordination results in an enhanced M 50 of 0.88 μ B /f.u. while suppressing H C to 0.01 kOe, indicative of a switch from antiferromagnetic-dominated to ferromagnetic-dominated magnetic interactions at organic/inorganic interfaces. First-principles calculations confirm the interfacial coordination-dependent magnetism, where the magnetization may further increase to ∼1.1 μ B /f.u. Interfacial modification also induces obvious changes in semiconducting properties, including a maximum blue shift of 10 nm in a photoluminescence emission response at interfaces. This study offers a foundation for developing advanced organic magnetic semiconductors for room-temperature applications.

CAS / MDL: 14024-18-1 7446-08-4
研究领域: 材料科学 · 凝聚态物理 · 无机化学 · 有机电子学 · 自旋电子学
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