CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wenhui Fang,Tingting Tang,Min Li,Shixian Xin,Ying Wu,Yutao Cao,Zhize Yu,Wei Cui,Zengxi Li,Hong Zhao
Designing catalysts at atomic level fine-tune the electronic structure of surface-active site for efficient water splitting, is a highly desirable approach but also poses significant challenges. This study focuses on the synthesis of a series of electronically tunable metal single-atom (M−SAs) catalysts: M 9 @S-Ni(OH) 2 (M=Pt, Mn, Fe or Cu). Experimental results reveal that introduction of trace S-heteroatoms and metal atoms into Ni(OH) 2 lattice can effectively modulate the electronic structure of M 9 @S-Ni(OH) 2 through modulation of p-d and d-d orbital hybridization, resulting in exceptional performance in water electrolysis. Among M 9 @S-Ni(OH) 2 , Pt 9 @S-Ni(OH) 2 and Fe 9 @S-Ni(OH) 2 exhibit excellent hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance, respectively, the overpotential requiring only 7 mV and 269 mV, respectively, at current density of 10 mA cm −2 . (−) Pt 9 @S-Ni(OH) 2 ||Fe 9 @S-Ni(OH) 2 (+) presents a high current density of 531.07 mA cm −2 at cell-voltage of 1.80 V in overall-water splitting (OWS), which is 14.07 times higher than that of the commercial (−) Pt/C||IrO 2 (+) (37.86 mA cm −2 ) system. This work achieves the development of cost-effective and stable electrocatalysts, offering a solution for large-scale and sustainable water-hydrogen conversion.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xinwei Xie,Yaoliang Huang,Li Xu,Guangyu Luo,Haifeng Liu,Xinlong Zhang,Jinyue Yang,Junze Lei,Xiaoyuan Yu
O3-type Ni/Mn-based transition metal oxides have garnered significant interest as cathode materials for sodium-ion batteries (SIBs) due to their high specific capacity and abundant resources. However, their commercialization application has been impeded by rapid capacity fading owing to structural degradation, gas evolution, irreversible phase transitions during charge/discharge cycling. Herein, The Zr 4 + /F - dual-doped strategy is developed to boost the Na-storage performance of Ni/Mn-based O3-NaNi 0.3 Fe 0.1 Mn 0.47 Cu 0.1 Zr 0.03 O 2-x F x (NFMCZF-x) layered oxide cathode material prepared by high temperature calcination method. Structural and electrochemical analyses reveal that Zr⁴⁺ doping expands Na⁺-layer spacing and F⁻ doping strengthens transition metal-oxygen bonds. These synergistic effects of Zr 4+ /F - dual-doping is benefit to suppressing O3↔P3 phase transitions, Jahn-Teller distortion and irreversible oxygen redox. Thus, the optimized NFMCZF-0.03 cathode delivers high specific capacity (178 mAh g −1 at 0.1 C) and excellent cycling stability (72 % capacity retention after 100 cycles at 1.0 C). This study establishes dual doping as an effective strategy for developing Ni/Mn-based layered oxide as high-performance cathodes for SIBs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
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IF 5.091
Hui Li,Ziqun Wang,Yunhui He,Sugang Meng,Yun Xu,Shifu Chen,Xianliang Fu
Rational synthesis of photocatalytic materials is an effective way to improve their performance. In this work, to optimize the S precursors, a series of Mn x Cd 1−x S (MCS) were first hydrothermally synthesized with the prevalent thiourea (TA), thioacetamide (TAA) and L-cysteine (L-Cys) as the S sources. The optimum feed ratio of Mn/Cd was then determined based on the optimized S precursor. The effects of S precursors and the feed ratio of Mn/Cd on the phase structure, absorption, morphology, band structure, and the photocatalytic hydrogen evolution reaction (HER) performance of MCS were investigated systematically. The hexagonal phase structures of MnS, CdS, and MCS are favored by TA and L-Cys as the S sources, while their cubic phases are benefited by TAA. TAA is the preferred S source for the preparation of highly active MCS and the solid solution is formed through the consolidation of cubic α-MnS into cubic CdS. The activity of MCS can be improved with the increase of Mn content from x = 0–0.6. The sample with x = 0.6 shows the highest HER activity (2253 μmol·h −1 ·g −1 ) and the performance is almost 6 times higher than CdS (416 μmol·h −1 ·g −1 ). The enhanced activity can be attributed to the improved separation efficiency of photo-induced charge carriers and the negative-shifts of E cb , which are induced by the introduction of Mn. A segregation of inert α−MnS from MCS is occurred when Mn content is >0.6, resulting in a decay of the HER activity. A change of the semiconductivity from n-type to bipolar type is occurred in MCS due to the uneven sulfidation of Mn in MCS.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Qi Zhang,Wei Li,Siyuan Cao,Xu Yin,Hongwei Zhu,Liankai Gu,Haoming Chen,Xiaoyuan Zhang,Weiqing Han,Kajia Wei
Precisely controlling atomic occupancy in edge-sharing sites remains challenging and limits the application of spinel oxides in advanced oxidation processes (AOPs). Herein, a series of inverse spinel oxides featuring edge-sharing Co Oh -O-Mn Oh (Oh means octahedral) configurations were designed to leverage inter-octahedral electronic redistribution and spin-state modulation, thereby enhancing catalytic performance for peroxymonosulfate (PMS) activation and pollutant degradation. The energy redistribution induced by this structure enhances the O-p/Mn-d orbital hybridization, accelerates the electron transfer kinetics between Co and Mn, and promotes the generation of high-valent cobalt-oxo (Co IV =O) species and singlet oxygen ( 1 O 2 ), thereby increasing the degradation efficiency of organic pollutants. The optimized Co-Mn inverse spinel achieved complete BPA removal within 15 min, exhibiting 11.4-fold enhancement in PMS activation efficiency than unmodified cobalt oxide, and with < 6.5 % average efficiency deviation at 100 mM ionic concentration. This study offers a strategy for the precise design of edge-sharing reactive sites in inverse spinel oxides and their application in AOPs.
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Journal of Materials Research and Technology-JMR&T
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2023
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IF 6.4
Jianwei Gao,Xiaoqing Si,Hanyue Ding,Xiaoyang Wang,Mushi Zheng,Chun Li,Junlei Qi,Jian Cao
Glass/Glass-ceramic sealing is always accompanied by issues of high porosity and brittle joints. To migrate these problems, an Ag foam was innovatively induced as an interlayer in the process of glass sealing the yttria-stabilized zirconia (YSZ) ceramic to Mn–Co spinel-coated Crofer 22 H stainless steel. Interlayer-added joints showed a significant reduction in porosity, and the shear strength was improved to 52.3 MPa, with an enhancement of 37.8 %. The influence of interlayer on the microstructure of the joint has been investigated and the formation process of the joint is illustrated. The Ag interlayer expels gases from the sealant material through expansion at high temperatures and promotes finer nucleation grains of crystallites integrating with the interlayer, reducing the porosity and alleviating the brittleness as well.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Haiyang Xie,Yuhan Chen,Xianni Li,Xiaoling Lu,Hao Lin,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
The selective oxidation of benzyl alcohol (BzOH) to benzaldehyde (BzH) is one of the effective methods for synthesizing chlorine-free benzaldehyde, but developing an efficient catalytic system remains a challenge. The peroxymonosulfate (PMS) is an inexpensive and soluble solid oxidant that has been widely used in oxidation reactions in aqueous media, however, there are still difficulties in activating PMS using atomically dispersed metal catalysts based on non-free radical pathways. Herein, an atomically dispersed manganese catalyst (Mn 1 /NLC), featuring electron-deficient Mn–N 2 O 2 sites anchored on a nitrogen and oxygen co-doped carbon support, is synthesized through a combined process of ball milling and high-temperature pyrolysis. The Mn 1 /NLC catalyst exhibits outstanding performance in the selective oxidation of BzOH to BzH by efficiently activating PMS, achieving 98.5% BzOH conversion and 99.2% BzH selectivity with a high turnover frequency of 1470.6 h −1 within 3 h at a PMS dosage of 10 mg and 45 °C, which surpasses the majority of the reported catalysts. Electron paramagnetic resonance, radical quenching experiments, and electrochemical analysis collectively reveal that the Mn–N 2 O 2 reaction sites lead to the formation of a high-valent Mn species, which enhances the adsorption of C H bonds and activation of PMS to significantly promote the occurrence of non-radical oxidation pathway, including singlet oxygen ( 1 O 2 ) generation and electron transfer processes (ETP). The synergistic effect of 1 O 2 and ETP enables Mn 1 /NLC to perform efficient and selective C H oxidation of various aromatic alcohols under mild conditions, while also demonstrating excellent cycling stability. This study provides a novel strategy for the design of high-performance atomically dispersed metal catalysts for the selective oxidation of aromatic alcohols.
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CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Qiang Liu,Yan-Jiang Liu,Hao-Tian Tong,Shi-Xiao Wei,Ting-Liang Xie,Shuang-Feng Yin
Co-free manganese-based Prussian blue analogues (Mn-PBAs) have emerged as exceptionally promising cathode materials for sodium-ion batteries (SIBs), offering low cost and high specific capacity. However, the detrimental Jahn-Teller effect, compounded by sluggish Na + diffusion kinetics and inherently poor electrical conductivity, severely undermines structural stability and cycling performance. Herein, we pioneer a novel Co-free entropy regulation strategy to overcome these formidable challenges. Four distinct Co-free PBAs with precisely controlled (configuration entropy (Δ S conf ) were meticulously synthesized via a straightforward co-precipitation method. Comprehensive electrochemical diagnostics combined with rigorous density functional theory (DFT) simulations unequivocally reveal that elevating Δ S conf demonstrably accelerates Na + diffusion, significantly enhances electrical conductivity, and effectively suppresses Jahn-Teller distortion. In situ X-ray diffraction (XRD) and in situ Raman spectroscopy analyses vividly characterized the structural transitions occurring during sodiation/desodiation, demonstrating markedly improved structural reversibility with increasing Δ S conf . Consequently, the Co-free high-entropy (HE) PBA cathode delivers truly remarkable cycling stability, (retaining 62.3 % capacity after an astounding 10 000 cycles at 5 000 mA g −1 , alongside exceptional rate capability of 75.1 mAh g −1 at 5 000 mA g −1 ). These groundbreaking findings provide profound insight for designing future high-performance cathode materials from abundant, environmentally friendly elements for next-generation SIBs.
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CHEMICAL ENGINEERING SCIENCE
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2026
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IF 4.3
Ruxin Liu,Tao Yu,Xingwang Niu,Jinsheng Li,Xuefei Lei,Zhaobo Wang,Rui Guo
Antibiotic pollution from compounds such as tetracycline hydrochloride (TC-HCl) is a growing concern due to its persistence in the environment and potential to promote antimicrobial resistance. Conventional treatment methods for such wastewater often suffer from low efficiency and high operational costs. In this study, a bimetallic FeMn-BTC material with a two-dimensional sheet-like morphology was synthesized via a facile one-pot ultrasonic method for the efficient degradation of TC-HCl. By precisely selecting the Fe/Mn molar ratio to 7:3, a high density of accessible Fe(II) active sites was achieved. Under visible-light irradiation, FeMn-BTC degraded 92% of high-concentration TC-HCl (100 mg/L) with a reaction rate constant of 0.06703 min −1 , which is 10.5 times higher than that of the monometallic Fe-BTC. This remarkable enhancement is attributed to the incorporation of manganese, which facilitates the Fe(III)/Fe(II) redox cycle and extends the visible-light absorption range. Density functional theory (DFT) calculations further verify that manganese doping lowers both the adsorption and O-O bond cleavage energy barriers of H 2 O 2 . Mechanistic studies identify hydroxyl radicals (·OH) as the primary reactive species, with the synergistic interaction between iron and manganese promoting H 2 O 2 activation and charge-carrier separation. The catalyst also exhibits excellent stability over a wide pH range (3–9) and shows universal degradation activity toward various pollutants (methylene blue, rhodamine B, and malachite green) as well as in real water matrices containing common anions such as Cl − and SO 4 2− . After four consecutive recycling runs, the material retains over 75% of its initial degradation efficiency, outperforming most reported metal–organic framework-based catalysts. This work offers theoretical insights and a practical strategy for designing highly efficient photocatalysts for Fenton-like reactions.
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OPTICAL MATERIALS
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2022
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IF 3.754
Rui Zhang,Gang Chen,Haiyun Liu,Jianfeng Zhang,Yaoxin Yuan,Zehua Lv,Lifu Zhang,Chunlan Wang,Zhenxing Qin,Wen Yang,Jinbin Wang
Doping Mn 2+ ions into cesium lead halide CsPbX 3 (X = Cl, Br, I) perovskite nanocrystals (PNCs) has been proven to be an effective strategy to reduce the Pb 2+ content. However, excessive Mn 2+ ions may form the Mn–Mn dimers in PNCs, leading to concentration quenching effects and low photoluminescence quantum yields (PLQYs). Herein, secondary metal ions (Ni 2+ , Cu 2+ , Zn 2+ ) were introduced to substitute Pb 2+ ions as co-doped (Mn, M):CsPbCl 3 PNCs (M = Ni, Cu, Zn), which were prepared by a facile method under ambient conditions, aiming for positively passivating the surface defects and improving the Mn 2+ emission. Also, to protect the co-doped (Mn, M):CsPbCl 3 PNCs from moisture damage, we performed silica encapsulation, which further passivated surface defects due to the effective hydrolysis of silane . The evolution of optical properties and stabilities of three series of (Mn, M):CsPbCl 3 PNCs was compared. The PLQYs of co-doped (Mn, M):CsPbCl 3 PNCs were larger than those of single-doped Mn: CsPbCl 3 PNCs, especially for (Mn, Ni):CsPbCl 3 and (Mn, Cu):CsPbCl 3 , which can reach nearly 30%. The PLQYs of (Mn, Ni):CsPbCl 3 and (Mn, Zn):CsPbCl 3 PNCs decreased dramatically during the encapsulation process, while the PLQY values of (Mn, Cu):CsPbCl 3 remained 30% even after the same treatment process. Consequently, the prototypes of white light-emitting devices (WLEDs) were successfully fabricated based on orange-red (Mn, Ni):CsPbCl 3 @SiO 2 and (Mn, Zn):CsPbCl 3 @SiO 2 composites. The synergetic effects of co-doping transition metal ions and silica-shell coating on improving optical properties and stabilities were investigated. It has potential for a wide range of applications in the field of solid-state light emission.
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高影响因子
APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Yaoliang Huang,Yunru Zhang,Guizhi Yuan,Dingshan Ruan,Xinlong Zhang,Weijian Liu,Zhongshuai Zhang,Xiaoyuan Yu
Ni/Mn-based layered oxides have been widely studied for sodium ion battery cathode because of high capacity and simple preparation. However, its application has been restricted owing to unstable structure and poor cycling performance. Herein, the multi-element doped hexagonal sheet Ni/Mn-based layered oxide with ZrO 2 surface modification O3-NaNi 0.3 Mn 0.5-x Fe 0.1 Cu 0.1 Zr x O 2 @ZrO 2 (NFMCZ-x) cathode materials have been successfully synthesize by high temperature calcination method accompanied by ball milling activation. XRD refinement results show Zr 4+ substitution of Mn 3+ can increase interlayer distance of sodium layer. Benefiting from the synergetic effect of multi-element doping and ZrO 2 surface modification, the optimized NFMCZ-0.03 sample exhibits a higher discharge capacity of 178 mAh/g at 0.1C and good capacity retention (77 % after 50 cycles at 2C). Furthermore, NFMCZ-0.03 has an excellent air stability with a capacity retention rate of 86 % during 50 cycles at 1C after being exposed in the air for 20 days. The ex-situ XRD results of NMFC at different charge/discharge voltages show Zr 4+ doping can suppress O3 + P3′'–O3′-O3 + P3′' phase transition during charge/discharge process. These results confirm that synergistic effect of multi-doping combined with surface modification can improve electrochemical performance of layered oxides cathodes, which provides a research idea for development of Ni/Mn-based layered oxides cathodes for sodium-ion batteries.
研究领域:
材料科学
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电化学
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能源存储
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无机化学
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固态化学
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高影响因子
OPTICAL MATERIALS
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2022
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IF 3.754
Yang Wang,Sheng Feng,Changchang Ma,Yun Zhou,Zhiwei Ye,Xiaojun Dai,Xun Cao
In this paper, a novel Mn-doped CdS@NH 2 -MIL-125(Ti) (MC@NT) photocatalytic composites was synthetized through hydrothermal method . Hydrogen desorption and tetracycline and oxytetracycline degradation were performed under visible light to test their photocatalytic activities . The composites were characterized by XRD , FTIR, SEM, TEM, XPS , UV–Vis diffuse reflectance spectroscopy (DRS), EPR , EIS, and transient photocurrent response. From the characterization consequence, it could be seen that Mn-doped CdS was tightly attached to the surface of tetragonal NT in the form of nanoparticles . The MC@NT composites exhibited more promising catalytic activity than pristine monomeric materials. The photocatalytic hydrogen evolution rate reached 3.61 mmol g −1 h −1 . Within 110 min, the degradation efficiencies of TC and OTC were 90% and 88%, respectively. The free radical trapping experiments proved that ·O 2 − and h + were decisive role for degrading pollutants in the degradation catalysis process. Radical trapping experiments and electron spin resonance (ESR) indicated that the Z-scheme heterojunction was formed between Mn-doped CdS and NT, leading to facilitate the migration and shift of photogenerated carriers and holes. Cycling experiments showed that the as-prepared composites have good stability and have good prospects for practical applications. We believe this work will offer new ideas on the future development of efficient heterojunction catalysts for light energy conversion and other applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yang Zong,Yufei Shao,Wenjie Ji,Yunqiao Zeng,Jun Xu,Wen Liu,Longqian Xu,Deli Wu
Traditional advanced oxidation processes (AOPs) generally suffer from the inevitable deactivation of catalysts and the ineffective consumption of transient reactive species (TRSs) that compromise the efficiency in destructing aqueous contaminants. Herein, it was interestingly found that trace Mn(II) could robustly catalyze the oxidation of organic contaminants by periodate (PI), with the performance was much better than the representative TRSs-dominated AOPs (i.e., the Fe(II)-activated hydrogen peroxide, peroxymonosulfate (PMS), peroxydisulfate and PI processes). Multiple lines of evidence excluded the oxidative contributions of TRSs, instead the stoichiometric formation of colloidal MnO 2 via the condensation of di-μ-oxo-bridged Mn(IV) cluster was confirmed by UV-vis, X-ray absorption near edge structure spectroscopy and density functional theory calculation. Dependent on the structure of substrate, MnO 2 colloids solely or simultaneously served as oxidant and catalyst for the enhanced treatment performance. Benefiting from the non-TRSs-involved oxidation strategy and the catalytic effects of Mn species, the trace-Mn(II)/PI process even outperformed the Co(II)-activated PMS counterpart (i.e., one of the most efficient AOPs known at present) on oxidant utilization efficiency. This study not only elucidated the roles of Mn(II) and colloidal MnO 2 in PI-mediated contaminant degradation, but also signified the superiority of trace catalyst-assisted process without TRSs involvement in avoiding undesired side reactions and maximizing oxidation efficiency.
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