CATALYSIS LETTERS
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2025
·Vol. 155
·期 9
·1-12
·
IF 2.4
Zhong Yuhang,Xu Hui,Li Zhiguo,Zhang Yuqi,Hou Jianyuan,Yuan Yuan,Liu Xingang,Zhang Renxi
This study demonstrates an innovative approach for green and efficient hydrogen production from seawater, utilizing Cu–Fe/Al 2 O 3 catalysts coupled with a dielectric barrier discharge (DBD) system. The catalytic performance was systematically evaluated under varying voltages and Cu/Fe ratios in a DBD reactor to optimize hydrogen production efficiency. Subsequent investigations focused on humidity and gas flow rate effects using the optimal catalyst (Cu/Fe/Al 2 O 3 = 2:1:9). Multimodal characterization (XRD, XPS, FTIR, OES) combined with DFT calculations revealed the mechanistic role of Cu–Fe/Al 2 O 3 in plasma-driven hydrogen generation. The synergistic interaction between Fe and Cu enhanced hydroxyl/hydrogen radical generation through improved adsorption, thereby boosting hydrogen evolution efficiency and yield. The optimized system achieved a maximum hydrogen yield of 7.4 g/kWh at 3 kV operating voltage, 3 L/min argon flow, and 100% relative humidity, establishing an energy-efficient pathway for sustainable hydrogen production from seawater. Graphical
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Yushi Han,Qin Yin,Shuo Geng
The development of the liquor industry urgently needs to solve the problem of wastewater treatment. The electrochemical oxidation method, with its advantages of high efficiency and environmental friendliness, has surpassed traditional processes. The low electro-oxidation potential of organic alcohols in wastewater (significantly lower than the oxygen evolution reaction, OER) endows it with dual value: it can replace the anode OER while simultaneously achieving pollutant degradation and driving the hydrogen evolution reaction (HER) at the cathode, achieving the synergy of “anode pollution control and cathode hydrogen production”. Based on this, this study constructed a Fe-NiOOH/NiMo/NF heterojunction catalyst, which, through the synergy of the efficient alcohol degradation ability of Fe-NiOOH and the excellent hydrogen evolution performance of NiMo, established a stable coupling system for wastewater degradation and hydrogen evolution at high current densities. Experiments confirmed that: Experimentally, the Fe-NiOOH/NiMo/NF anode delivers 200 mA cm −2 at 1.434 V vs. RHE; the NiMo/NF cathode reaches 20 mA cm −2 at an overpotential of 88 mV; and the full cell (Fe-NiOOH/NiMo/NF=|NiMo/NF) sustains 100 mA cm −2 for 100 h with only a 30 mV rise in voltage. Compared with the high-purity alcohol-based OER replacement scheme, using low-cost liquor wastewater as the anode reactant significantly reduces the cost of hydrogen production. The stable operation of this synergy system at high current densities provides a reliable technical path for the industrialized wastewater degradation and hydrogen production.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Yu Shao,Zhisheng Mao,Jiarui Wang,Xianfeng Hao,Yongchao Jia,Yuanhui Xu,Keju Sun
The electrochemical synthesis of hydrogen peroxide through two-electron oxygen reduction (2e– ORR) presents a sustainable alternative to conventional synthesis methods, such as the anthraquinone method. TiO2-based materials are promising candidates due to their stability and tunable electronic properties, but their intrinsic 2e– ORR activity and selectivity are insufficient for practical applications. Here, we report that strategic Fe doping significantly enhances the 2e– ORR performance of TiO2. The optimized Fe-TiO2 catalyst exhibits remarkable activity and selectivity, achieving a 30% increase in H2O2 selectivity (from 47% to 77%) while reducing the electron transfer number from 3.05 to 2.45 in 0.1 M KOH electrolyte. Notably, the material shows substantially improved electrochemical active surface area (ECSA) and ORR kinetics, culminating in an exceptional H2O2 production rate of 406 mmol·gcat–1·h–1 with 97.5% Faraday efficiency at 0 V vs RHE in an H-cell configuration. Density functional theory (DFT) calculations reveal the mechanistic origins of this enhancement: Fe doping effectively narrows the band gap and lowers the oxygen vacancy formation energy, thereby boosting electrical conductivity as confirmed by experimental characterization; and the modified electronic structure increases Bader charge accumulation on the terminal oxygen of adsorbed *OOH intermediates, facilitating protonation at this site and consequently promoting the 2e– pathway. These dual effects synergistically enhance both ORR activity and H2O2 selectivity. This study not only presents Fe-TiO2 as an efficient, earth-abundant catalyst for sustainable H2O2 production but also establishes fundamental design principles for developing advanced metal oxide electrocatalysts through targeted heteroatom doping.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Guanhong Liu,Rongze Tang,Congcong Wang,Dehong Yu,Zhenxin Wang,Haochen Yang,Jia Wei,Shunhua Zhu,Fenglei Gao,Feng Yuan,Bin Pan
Cuproptosis and ferroptosis are difficult to synergize in tumor suppression due to their spatiotemporal asynchrony and mechanistic dispersion. Therefore, we proposed a new paradigm of Ferroptosis-Cuproptosis self-recycling. An iron‑sulfur cluster (Fe-S) metabolic collapse was constructed by hyaluronic acid (HA)-functionalized bimetallic nano-enzymes (HA@CuCo-NC) to initiate this tumoricidal mechanism. HA@CuCo-NC specifically accumulates in osteosarcoma cells through HA-mediated targeting. The multi-enzyme activity triggers a surge of reactive oxygen species (ROS) in the tumor microenvironment, which, along with Co 2+ , induces ferroptosis. This leads to severe mitochondrial damage and glutathione (GSH) depletion, which in turn activates the cuproptosis cascade. Cuproptosis causes Fe-S protein degradation and Fe 2+ release into the labile iron pool (LIP) by inhibiting Fe-S cluster formation and dihydrolipoamide acetyltransferase (DLAT) oligomerization. The released Fe 2+ enhances oxidative stress and promotes membrane disassembly via the Fenton reaction. The two act synergistically to form a dynamic self-reinforcing cycle: Ferroptosis-related mitochondrial damage exacerbates the toxicity of Cu 2+ . Cuproptosis-released Fe 2+ further activates ferroptosis. In vivo experiments demonstrated that HA@CuCo-NC significantly inhibited the growth of osteosarcoma in situ without causing systemic toxicity. This research introduces a novel approach to treating solid tumors by reconstructing the metabolic interaction network of copper and iron.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Wenwen Yin,Jiawei Ma,Yanyan Li,Qing Cheng,Bernt Johannessen,Fangxi Xie,Mingmei Wu
Exploiting bifunctional and highly efficient electrocatalysts that can facilitate the reversible formation and decomposition of discharge products is crucial for rechargeable Na-air batteries (SABs). However, restricted by scaling relations, air cathodes based on single metal systems usually exhibit inferior activity and fail to achieve a stable and long cycle life of Na-air batteries. Dual single-atom catalysts (DACs) with two metal sites can circumvent the scaling relations and endow the single-atom catalysts with superior activity. Herein, we present a hollow carbon microsphere loaded with Ni and Fe single atoms (Ni-HCMs-Fe) as a demonstration of DAC air cathodes for SABs. Notably, Na-air batteries with Ni-HCMs-Fe as an air cathode can achieve a low overpotential gap of 530 mV, a high specific capacity of 5382.9 mAh g−1, and an ultralong cycle life of over 450 cycles (1800 hours) with NaO2 as the main discharge product. Due to the different adsorption energies between oxygenated intermediates and Ni/Fe sites, the Ni-HCMs-Fe catalysts can break through the scaling relations and display optimized binding ability towards intermediates, thus boosting the reversible formation and decomposition of NaO2 in SABs. This work pioneers the use of DACs in SABs, paving the way for their practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Yunxiao Zheng,Xiaohui Wu,Yongchun Zhao,Tao Zhou,Mingjie Huang
Polymerization transfer (PT) technology is highly advantageous for treating high-salinity wastewater due to its high tolerance to coexisting anions and superior electron utilization efficiency. Here, we report the unusual simultaneous achievement of rapid pollutant removal (pseudo-first-order rate constant of 0.15 min −1 , 56.0-fold higher than unmodified counterparts) and high PT ratio (>65 %) in a peroxymonosulfate (PMS) activation system. This was achieved by simply tuning the Fe content within a rationally designed Fe/N engineered pine sawdust biochar catalyst. Performance enhancement stems from Fe-induced graphitization improving electron transfer, coupled with N-induced moderate orbital hybridization between Fe 3 d (Fe/N biochar) and O 2 p (PMS) atomic states, optimizing PMS adsorption-desorption and yielding the lowest energy barrier for Fe(IV) O formation. Remarkably, the system maintains robust performance under high salinity conditions (500 mM Cl − , HCO 3 − , NO 3 − , and SO 4 2− ) and achieves 67.5–77.3 % chemical oxygen demand (COD) removal during 17-day continuous-flow treatment of real coking wastewater, where polymerization-mediated organic removal through C C/C O coupling. Furthermore, residual oligomers are efficiently removed by subsequent activated carbon (AC) adsorption or poly-ferric sulfate (PFS) coagulation, establishing an integrated “catalytic polymerization-AC/PFS polishing” paradigm for sustainable treatment of refractory organics in high salinity coking wastewater.
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MICROCHEMICAL JOURNAL
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2025
·
IF 5.1
Junjie Qi,Wenhui Hao,Jingkun Li,Yuqi Wan,Guoyong Jiang,Yukihiro Ozaki,Fuwei Pi
Phoxim is a broad-spectrum organophosphorus pesticide widely used in the world; however, its neurotoxicity and potential risk pose a significant threat to human health and ecosystems. To address this issue, based on the same metal clusters and similar topologies, a MOF-on-MOF composite strategy, i.e., PCN222(Fe)@NU-1000, was developed for rapid evaluation of phoxim via ratiometric fluorescence and colorimetric dual-signal output. Herein, the inner core, PCN222(Fe), imparts peroxidase-like catalytic activity enabling colorimetric detection based on the 3,3′,5,5′-tetramethylbenzidine (TMB) and the solution decolourisation caused by acetylcholinesterase (AChE) products, while the outer shell, NU-1000, provides a strong fluorescence emission at 461 nm. This core-shell structure also facilitates fluorescence resonance energy transfer (FRET), whereby phoxim selectively quenches the fluorescence of NU-1000 without affecting PCN222(Fe), enabling ratiometric fluorescence sensing. This integrated dual-signal system-comprising ratiometric fluorescence and enzyme-mimetic colorimetry-ensures signal cross-verification and improved detection accuracy. The fluorescence mode exhibits a quantification range of 5.0 ng/mL to 4.0 μg/mL with a detection limit of 4.0 ng/mL, while the colorimetric mode shows a linear range from 2.5 ng/mL to 25.0 ng/mL and a detection limit of 1.76 ng/mL. Furthermore, the method accurately evaluates phoxim levels in fruits and vegetables such as apples and celery, achieving recoveries ranging from 95 % to 115 % and a relative standard deviation (RSD) of less than 9 %. This MOF-on-MOF dual-signal sensing strategy is designed to be simple, user-friendly, and highly reliable, providing significant value for the development of rapid and sensitive approaches in food and environmental science.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 10
·1-13
·
IF 5.3
Meng Dongling,Chen Zhiyan,Chen Zhibin,Cen Junrao,Li Jitao,Yang Yaling
Iron-cerium co-doped carbon dots (Fe,Ce-CDs) were synthesized by one-step hydrothermal method using tartaric acid and L-tryptophan as ligands. Fe,Ce-CDs shows excellent peroxidase-like (POD) activity and nitrite (NO 2 − ) can promote the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to its blue oxidation product (oxTMB) due to the formation of ∙NO 2 free radical. NO 2 − further react with oxTMB to form a yellow color via diazotization resulting in the absorbance Change at 450 nm. By Fe,Ce-CDs + NO 2 − + TMB + H 2 O 2 and oxTMB + NO 2 − systems, a dual-signal colorimetric nanosensor for NO 2 − detection is developed with lower detection limits (LODs) of 0.272 μg/L and 0.019 mg/L, respectively. The proposed methods were applied to the detection of NO 2 − in tobacco samples with good recovery from 91.20 to 110.61%, achieving similar results and indicating their high accuracy and feasibility. Graphical
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Hongying Sha,Yuxuan Feng,Jingbo Mao,Hui Lv,Jinxia Zhou
The hydrodeoxygenation of lignin-derived syringol to phenol faces challenges in selectively cleaving C Aryl –O bonds while maintaining aromatic ring and a phenolic -OH group integrity. Herein, we developed a trimetallic CoFeAg/SiO 2 catalyst that achieves 100 % syringol conversion and 52.4 % phenol selectivity, surpassing bimetallic CoAg/SiO 2 (42.2 mol%) and monometallic Co/SiO 2 (7.6 mol%) catalysts. As promoters, Ag facilitates the low-temperature reduction of Co 3 O 4 to CoO and further to metallic Co, while Fe prevents excessive reduction of CoO to metallic Co. Through the synergistic effects of Fe and Ag on Co, the CoFeAg/SiO 2 catalyst undergoes in situ reduction under reaction conditions (1 MPa H 2 , 330 °C), forming a polycrystalline CoO-Co structure with abundant oxygen vacancy (O ᴠ ) and Lewis acid sites. The CoO-Co-O v active sites facilitate heterolytic H 2 cleavage while preferentially adsorbing and activating oxygen-containing functional groups over the aromatic ring of syringol. This dual functionality selectively promotes C Aryl –O bond dissociation while suppressing undesired ring hydrogenation, providing an effective catalyst design strategy for sustainable phenol production from biomass-derived syringol.
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Journal of Energy Chemistry
·
2024
·
IF 14
Jiawen Wu,Yuanzhi Zhu,An Cai,Xiaobin Fan,Wenchao Peng,Yang Li
Fe-N-C catalysts are widely considered as promising non-precious-metal candidates for electrocatalytic oxygen reduction reaction (ORR). Yet despite their high catalytic activity through rational modulation, challenges remain in their low site density and unsatisfactory mass transfer structure. Herein, we present a structural engineering approach employing a soft-template coating strategy to fabricate a hollow and hierarchically porous N-doped carbon framework anchored with atomically dispersed Fe sites (FeNC-h) as an efficient ORR catalyst. The combination of hierarchical porosity and high exterior surface area is proven crucial for exposing more active sites, which gives rise to a remarkable ORR performance with a half-wave potential of 0.902 V in 0.1 M KOH and 0.814 V in 0.1 M HClO 4 , significantly outperforming its counterpart with solid structure and dominance of micropores (FeNC-s). The mass transfer property is revealed by in-situ electrochemical impedance spectroscopy (EIS) measurement. The distribution of relaxation time (DRT) analysis is further introduced to deconvolve the kinetic and mass transport processes, which demonstrates an alleviated mass transport resistance for FeNC-h, validating the effectiveness of structural engineering. This work not only provides an effective structural engineering approach but also contributes to the comprehensive mass transfer evaluation on advanced electrocatalyst for energy conversion applications.
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CHEMICAL PHYSICS
·
2024
·
IF 2
Qian Liu,Panpan Xu,Qianqian Zhang,Guangming Han,Ling Li,Limin Zhou
A series of novel MIL-53(Fe)/CoWO 4 composites were synthesized by combining MIL-53(Fe) and CoWO 4 nanoparticles via solvothermal method. The structural characterizations showed that CoWO 4 nanoparticles were uniformly distributed on the surface of hexagonal bipyramid MIL-53(Fe). Combining XPS and Mott-Schottky plots, a Z-scheme heterojunction was formed between MIL-53(Fe) and CoWO 4 , resulting in a significant improvement in the electron-hole pair separation efficiency. UV–vis diffused reflectance spectra indicated that the optical arrange of MIL-53(Fe)/CoWO 4 composites were expanded to visible light. The photocatalytic degradation experiments under visible light irradiation showed that MIL/CWO-60 synergistically with PMS degraded 90.5 % of TC-HCl within 50 min. The XRD spectra of used and unused composites were identical, indicating good stability in four consecutive cycles. Electron paramagnetic resonance (EPR) and free radicals trapping experiment revealed that active species included O 2− , SO 4 − , h + , OH and 1 O 2 , and mechanism of the synergistic degradation of TC-HCl by MIL-53(Fe)/CoWO 4 composites and PMS was proposed.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yourong Wu,Wanqian Cai,Shiqi Zhong,Cong Lin,Mei Lin,Tengfei Lin,Min Gao,Chunlin Zhao,Xiao Wu
Conventional nanomaterials are met with the bottleneck problem of difficult recycling and reuse when applied to water treatment. Carbon aerogel with three-dimensional structure can effectively solve the problem of recycling, however, the preparation of efficient and recyclable aerogel catalyst is still an urgent technical problem. Here, an NH 2 -MIL-88B(Fe)/agarose carbon aerogel (MGA-x) was synthesized at different calcination temperatures (x = 100, 150, 200 and 300 °C) and their changes in structures and photo-electrochemical properties were investigated. As a photo-Fenton catalyst, the aerogel could efficiently activate H 2 O 2 to ultrafast degrade mitoxantrone in water. Within 2 min, the removal efficiency of mitoxantrone in the MGA-200/H 2 O 2 /Light system was 97.6%, which was 85.3 times greater than that in the agarose aerogel/H 2 O 2 /Light system. Notably, the aerogel catalyst could be directly recovered and recycled without additional treatments, and the microstructure and degradation performance were maintained even after five cycles, demonstrating excellent sustainability for applications in practical aquatic environment. The primary active radicals involved in the photocatalytic degradation process were • OH, h + and • O 2 - , which were confirmed through free radical quenching experiments and electron paramagnetic resonance analysis. Additionally, possible degradation pathways for mitoxantrone were proposed based on the results of liquid chromatography-mass spectrometry. This study presents a photocatalytic aerogel with highly efficient degradation ability along with recycling and reuse capacity, exhibiting great potential for application in the remediation of water pollution.
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