Inorganic Chemistry Frontiers
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2026
·
IF 6.2
Shi-Yu Lu,Chuan Li,Longyu Qiu,Yan Zhang,Jiaming He,Minqi Liang,Xin Peng,Jun Zhang,Yin Liu,Juan Liu,Chuan Tan,Menggang Li,Meng Jin
Targeted regulation of electrocatalyst reconstruction during the oxygen evolution reaction (OER) under alkaline conditions proves essential to achieving highly efficient hydrogen production via electrochemical water splitting. Yet this remains a considerable challenge. Herein, we prepare an iron nickel phosphate (Fe-NPO) catalyst, which possesses substantial oxygen vacancies and an asymmetric Fe-O(P)-Ni coordination structure. This structural merit facilitates the effective deep reconstruction of Fe-NPO, which then transforms into the highly active Fe-Vo-P-NiOOH active phase during OER. For the reconstructed Fe-Vo-P-NiOOH, it effectively tunes the d-band center, bringing it notably closer to the Fermi level. This type of electronic modulation not only strengthens the water adsorption capacity but also optimizes the rate-determining step (RDS) in the OER pathway. The anion-exchange membrane water electrolyzer (AEMWE) integrated with the Fe-NPO catalyst as an anode catalyst achieved high industrial current densities of 500, 1000, 1500 and 2000 mA cm-2 at low applied voltages of 1.68, 1.76, 1.84 and 1.92 V, respectively. This work presents a strategy to realize the deep and efficient conversion of OER catalysts into highly active components through defect engineering and asymmetric coordination regulation, while also confirming Fe-NPO’s considerable potential for practical hydrogen production scenarios.
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Chemical Science
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2026
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IF 8.1
Wenlong Zhang,Xiaohui Ning
The Fe/FeCl₂-Graphite battery is an intermediate-temperature molten salt electrochemical system. It employs the solid Fe/Fe2+ redox as the negative electrode reactions and graphite positive electrode based on the intercalation/de-intercalation reaction of AlCl- 4, offering high safety, low material cost and a moderate operating temperature range of 110-150 °C. However, the poor electronic conductivity and high nucleation barrier in the FeCl2 material result in limited electrochemical reversibility and reaction kinetics. Here, we demonstrate that the Fe-FeCl₂ contact interface effectively enhances the redox reversibility and electrode kinetics by providing favorable sites for Fe⁰ nucleation and improving electronic conductivity. The prepared Fe-FeCl₂-CR electrode delivers low voltage hysteresis of 0.09 V and exhibits excellent electrochemical reversibility in the Fe/FeCl₂-graphite molten salt battery, achieving a specific capacity of 162.6 mAh g⁻¹ at 3 mA cm⁻² and retaining 93% of its capacity after 200 cycles. Compared with the pure FeCl₂ electrode, the Fe-FeCl₂-CR electrode shows lower direct‑current pulse resistance and negligible nucleation overpotential, which are primarily attributed to the Fe‑philic nucleation interface. This mechanism is further confirmed by density functional theory (DFT) calculations, revealing that the (110) crystal plane of nano‑Fe possesses the highest binding energy (-55.94 eV) during charging, thereby serving as the potential dominant interface for Fe⁰ nucleation. Additional self‑discharge and capacity expansion tests further confirm the electrochemical reaction stability of Fe-FeCl₂-CR electrode in Fe/FeCl₂-Graphite molten salt battery.
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Results in Chemistry
·
2025
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IF 4.2
Wei Zhang,Ku Yu,Wang Aihe
In this study, pyridine-a representative nitrogen-containing heterrocylic contaminant in coal chemical wastewater-was targeted for photocatalytic degradation. We developed a novel ternary composite photocatalyst through the in-situ integration of layered double hydroxide (LDH) and iron-based metal-organic framework (MIL-101(Fe)) with lanthanum‑iron co-doped TiO 2 via hydrothermal synthesis. These contaminants are characterized by high environmental persistence, low biodegradability, and potential teratogenic/carcinogenic risks. The synthesized LDH/MIL-101(Fe)/La-Fe-TiO 2 composite was systematically characterized using scanning electron microscopy (SEM), UV–Vis diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) analysis. Key findings revealed that: (1) The composite architecture achieves an exceptional specific surface area of 168.96 m 2 /g through synergistic LDH/MIL-101(Fe) integration; (2) La–Fe co-doping effectively extends the photoresponse threshold of TiO 2 to the visible-light region. Under optimized conditions (25 °C, 300 rpm agitation, 400 W irradiation), the system achieved 96.1 % pyridine degradation (initial concentration: 100 mg/L) within 4 h, following pseudo-first-order kinetics (R 2 = 0.99). Remarkably, the catalyst maintained 94.5 % efficiency after five consecutive cycles, demonstrating superior stability. Mechanistic investigations combining GC–MS analysis, electron paramagnetic resonance (EPR) detection, and radical quenching tests identified the reactive species activity sequence as ∙ h + > ∙ OH > O 2 − , ultimately elucidating the complete pyridine mineralization pathway.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Xiaofang Cao,Mingkai He,Baopeng Ma,Shixuan Liu,Xiaohui Pang,Mingzhen Song,Fudong Zhang,Xiaolian Chao,Zupei Yang,Di Wu
The band degeneracy thus thermoelectric performance of (Fe, Co)Sb 3 based p -type skutterudites can be well modulated by adjusting Co/Fe ratio. Combining systematic experiments and density function theory (DFT) calculations, we revealed in this work that the variation of Co/Fe ratio could result in complicated and mutually coupled effects on the individual thermoelectric parameters (band degeneracy, band gap, Fermi level , filling limit of fillers, phonon spectrum, etc.) and that using Co/Fe ratio to improve the overall thermoelectric figure of merit is nontrivial. We eventually found that the optimal Co/Fe ratio for Mm (Misch metal) filled (Fe, Co)Sb 3 lies at 1.3:2.7, which is somewhat off the Co/Fe = 1:3 point where the largest valence band degeneracy appears. Extra Sb was then introduced to compensate Sb volatilization for improved electrical transport performance. An overall peak figure of merit ZT max of 1.06 was eventually achieved in the sample Mm 0.8 Fe 2.7 Co 1.3 Sb 12.60 , which is among the highest ones for all reported (Fe, Co)Sb 3 based p -type skutterudites so far.
研究领域:
材料科学
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热电学
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凝聚态物理
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能源材料
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MICROCHIMICA ACTA
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2023
·Vol. 190
·期 5
·1-10
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IF 5.7
Wei Chunying,Lin Huiqing,Bai Hehe
Five G-/C-rich single-stranded DNA (ssDNA) with different sequences and lengths were templated to prepare the DNA-Cu, DNA-Fe, and bimetallic DNA-Cu/M nanoclusters (NCs). The peroxidase-like activities of these nanomaterials were studied using H 2 O 2 and 3,3′,5,5′'-tetramethylbenzidine (TMB) as the reaction substrates in HAc-NaAc buffer. It was found that T30-G2-Fe NCs and T30-G2-Cu/Fe NCs, with a size of about 2 nm, exhibit similar and the strongest enzyme-like activity under optimal conditions. Both NCs possess a similarly high affinity to substrates, and the Michaelis–Menten constant ( K m ) values to TMB and H 2 O 2 are about 11 and 2–3 times lower than those of natural horseradish peroxidase (HRP), respectively. The activity of both nanozymes decreases to about 70% after being kept for one week in pH 4.0 buffer at 4 °C, which is comparable with HRP. Hydroxyl radicals (•OH) are the main reactive oxygen species (ROS) produced in the catalytic reaction. Moreover, both NCs can facilitate in situ generation of ROS in HeLa cells using endogenous H 2 O 2 . MTT assays indicate that the T30-G2-Cu/Fe NCs exhibit the strong selective cytotoxicity to HeLa cells over HL-7702 cells. The cellular viability is about 70% and 50% after incubating with 0.6 M NCs for 24 h without or with 2 mM H 2 O 2 , respectively. The current study shows that the T30-G2-Cu/Fe NCs have the potential for chemical dynamic treatment (CDT). Graphical abstract
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2023
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IF 4.3
Yunxin Shi,Liying Wang,Xin Miao,Zhenzhu Cao,Yongfeng Zhang,Lin Cheng,Jucai Yang
A series of donut-like nanostructured heterojunction materials are first synthesized via one-step solvothermal method to improve the photocatalytic efficiency for the environmental pollutants. The unique donut-like Fe-doped-BiOCl@Fe-MOF heterojunction with uniform size guarantees suitable surface area and many active sites for the model pollutant. The optimal photocatalytic efficiency is shown in degradation of RhB (99.0 %, 90 min) and TC (90.4 %, 90 min) solution, which had higher photocatalytic efficiency than a variety of similar materials previously reported. The result revealed that the enhancing photocatalytic activity is mainly depended on the synergistic effect of Fe-MOF and Fe-doped BiOCl. The possible mechanism is further studied, which shown h + and O 2 − are the primary active species in the degradation process of RhB and TC solution. Meantime, Fe-doped BiOCl@Fe-MOF with the excellent reusability and stability. After the fourth cycle, the degradation rate of RhB solution can still be as high as 86.4 %. In this work, we provide a higher efficiency heterojunction photocatalytic material by varying the organic ligand content.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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CHEMOSPHERE
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2023
·
IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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WATER RESEARCH
·
2022
·
IF 13.4
Haolin Xu,Rundong Chen,Sheng Liang,Zhenchao Lei,Wenxiao Zheng,Zhang Yan,Jianxin Cao,Chaohai Wei,Chunhua Feng
The formation of chlorinated byproducts represents a significant threat to the quality of the effluent treated using electrochemical advanced oxidation processes (EAOPs), thus spurring investigation into alleviating their production. This study presents a new strategy to minimize the release of chlorinated intermediates during the electrochemical oxidation of Ni-EDTA by establishing a dual mixed metal oxide (MMO)/Fe anode system. The results indicate that the dual-anode system achieved a substantially higher rate (0.141 min − 1 ) of Ni-EDTA destruction and accordingly allowed a more pronounced removal of aqueous Ni (from 39.85 to 0.63 mg L − 1 ) after alkaline precipitation, compared with its single MMO anode (0.017 min − 1 of Ni-EDTA removal, with 14.38 mg L − 1 Ni remaining) and single Fe anode (insignificant Ni-EDTA removal, with 38.37 mg L − 1 Ni remaining) counterparts. Compared to reactive chlorine species (RCS) produced from the single MMO anode system, Fe(IV) was in situ generated from the dual-anode system and was predominantly responsible for the attenuation of chlorinated byproducts and thus the decrease in the acute toxicity of the treated solution (evaluated using luminescent bacteria). The Fe(IV)-dominated dual-anode system also exhibited superior performance in removing multiple pollutants (including organic ligands, Ni, and phosphite) in the real electroless plating effluent. The findings suggest that the strategy for Fe(II) transition to Fe(IV) by active chlorine paves a new avenue for yielding less chlorinated products with lower toxicity when EAOPs are used to treat chloride-containing organic wastewater.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Yibing Xie,Mengyu Wang,Xueqian Wang,Langlang Wang,Ping Ning,Yixing Ma,Jichang Lu,Rui Cao,Yu Xue
The traditional way for arsine (AsH 3 ) removal from the reducing exhaust gas by catalytic oxidation undershot the expect goal in pollutant emission control. This laboratory scale work used magnetic field to improve the chemical environment of AsH 3 catalytic oxidation over magnetic response catalyst Fe/HZSM-5. After introducing external magnetic field at a magnetic field intensity of 0.1 T, the catalytic performance of Fe/HZSM-5 for AsH 3 removal was improved by 52%, and the turnover frequency (TOF) value increased from 4.65 × 10 −3 s −1 to 5.73 × 10 −3 s −1 . The structure–activity relationship of the catalyst in the presence of magnetic field was investigated. The characterization results showed that Fe is mainly anchored onto the surface of Fe/HZSM-5 catalyst through an oxygen bridge, while a small proportion of Fe exists in the form of iron oxides . The Fe species and surface labile oxygen (O − ) in the aluminum tetrahedra are the magnetic active sites of Fe/HZSM-5, magnetic field promotes the reaction by increasing the activity of them. It was discovered that paramagnetic O − increased by 50% in the presence of magnetic field compared with that in its absence. Therefore, a magnetic-field-assisted oxygen cycling process is proposed. In terms of the stability of catalyst, formation of more amorphous oxidized arsenic after reaction in the presence of magnetic field reduced the toxicity to the strong acid sites of the catalyst, and the holding time of excellent AsH 3 removal efficiency was prolonged from 23 h to 35 h. These results provide new insights into magnetic-field-assisted zeolite catalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaobing Wang,Chengyu Wei,Xiaosheng Song,Zuohui Wang,Yong Zhao
In the oxygen evolution reaction (OER), the non-reversible destruction of surface electronic structure caused by the irregular element migration in complex surface/interface reaction limits the improvement of catalyst’s activity and stability. Herein, we successfully realize the control of ‘dual-path migration of metallic elements in OER’ to stepwise reconstruct the O-coordinated bi-metal heterodimer (M 1 -O-M 2 ) for electron density redistribution. By designing Fe@FeNi 3 @NiO-Fe 3 O 4 (F-FN-NFO) model electrode with stepwise surface treatment in OER process, the directional migration (from core to shell, path 1 ) and adjacent-surface migration of Fe atoms ( path 2 ) are both controlled to reduce the formation energy of Ni-O-Fe units, realizing strengthened electron transfer between heterogeneous metal centers. After the surface reconstruction, the OER activity of F-FN-NFO increases for 8.6 times at 1.7 V (30.5–263 mA cm −2 ). Based on this strategy, the designed three-dimension NiFe@NiFe x O is positive activated compared to traditional NiFe-oxidation with the overpotential reduced to 299 mV at 10 mA cm −2 .
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