EES Catalysis
·
2025
·
IF 8.1
Jie Yang,Lifang Chen,Xuya Zhu,Wenwen Shi,Mengxue Huang,Chang Liu,Ruimin Ding,Lin Gan,Xi Yin
H2O2 -related electrochemical reactions, including two-electron oxygen reduction reaction (2e-ORR), H2O2 oxidation reaction (HPOR), and H2O2 reduction reaction (HPRR), have received significant attention for the electrosynthesis H2O2 and energy storage. Understanding the complex structure-activity relationships among 2e-ORR/ HPOR/HPRR and their connections is crucial for further developing highly efficient catalysts and working systems. Herein, we unveil these intricacies by employing model Co-N-C catalysts with well-defined active site configuration (Co-N4-pyrrolic and Co-N4- pyridinic ) in a combined experimental and computational approach. We report the higher 2e-ORR/HPOR but lower HPRR activity of CoN4-pyrrolic site than the CoN4-pyridinic site based on their reaction free energy landscapes remodeled considering the chemisorption steps of O2 and H2O2 . The results reveal that the binding free energy of *OOH (ΔG*OOH ) can only be utilized as a reliable descriptor for 2e-ORR/HPOR activity, but not indicative of HPRR activity, regardless of the scaling relationship of the common reaction intermediates ( *OOH or *OH). The HPRR activity of CoN 4 sites strongly depends on the H2O2 adsorption strength and configuration. These findings provide valuable insights into the design of catalysts for H2O2 -related electrochemical energy conversion and storage systems.
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Industrial Chemistry & Materials
·
2025
·
IF 11.9
Rongkai Cui,Minlei Yin,Xiaoyan Chen,Xiaoyu Lou,Chen Yang,Ting Qiu,Jie Chen
To achieve sub-angstrom separation of N-methylpyrrolidone and 1,5-dimethyl-2-pyrrolidone, cyclodextrin-derived carbon materials with distinct pore environments and surface functionalities were synthesized via hydrothermal carbonization and high-temperature pyrolysis. Three types of carbons were obtained: non-porous carbons rich in surface functionalities, carbons with both functionalities and microporous structures, and carbons with limited functionalities but diverse micropore environments. Systematic adsorption experiments, supported by density functional theory and molecular dynamics simulations, were conducted to establish the structure–performance relationships. The results demonstrate that surface functionalities alone are insufficient for separation, whereas pore confinement is the decisive factor. A 7.3 Å pore was identified as the optimal confinement space, providing the strongest thermodynamic interactions and the fastest diffusion kinetics, thereby enabling highly selective adsorption of 1,5-dimethyl-2-pyrrolidone from N-methylpyrrolidone. This work not only clarifies the pore formation mechanism of cyclodextrin-derived carbons but also highlights precise pore-size tuning as a paradigm for sub-angstrom molecular separation, offering theoretical guidance for the design of advanced adsorbent materials.
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Sustainable Energy & Fuels
·
2025
·
IF 4.1
Yongheng Xiong,Yang Yu,Huangang Shi,Jifa Qu,Wenyi Tan
Single atom Fe sites, doped in CN materials, exhibit outstanding electrochemical activity for CO2-to-CO conversion. The pyrolysis of ZIF8 is a controllable method for fabricating isolated single atom metal sites. In this study, we propose a new strategy to increase the ratio of Fe in ZIF8 precursors by synergistically replacing Zn2+ with Bi3+ and Fe3+. After precursor pyrolysis, the obtained Bi/Fe–N–C catalysts, consisting of Bi sites and pyrrole-type Fe–Nx sites, serve as efficient electrocatalysts for the CO2RR. The results show that the optimized catalyst loaded with 94.8 mg per kgCat Fe exhibits a high FECO of >90.1% over a wide potential range of −0.4 to −0.7 VRHE (98.2% at −0.5 VRHE). Insights into the electrochemical reaction mechanism show that this successful design of Bi/Fe–N–C catalysts can provide a stable catalytic site to form *COOH, thus achieving energy-efficient electrochemical CO2 reduction to CO.
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JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Ma Junjie,Li Wei,Yang Deyi,Liu Zheng,Cao Yuyuan,Wang Shaocong,Han Guo-Cheng,Chen Qizhi
N-RGO/Na 3 V 2 (PO 4 ) 3 dual-modified Na 2 Fe 0.6 Mn 0.4 PO 4 F composites were prepared by sol–gel method combined with high-temperature calcination at 625 °C. Electrochemical tests show that the initial discharge specific capacity of N-RGO/Na 3 V 2 (PO 4 ) 3 -modified Na 2 Fe 0.6 Mn 0.4 PO 4 F composites is 149.27 mAh·g −1 at a current density of 0.05 C, and the discharge specific capacity can be maintained at approximately 101.89 mAh·g −1 after 100 cycles. This accounts for 68.26% of its initial discharge specific capacity. Rate performance tests showed that after cycling the current density back to 0.2 C, it was still able to recover to a discharge specific capacity close to 119 mAh·g −1 . At the same time, the interfacial properties of the N-RGO/Na 3 V 2 (PO 4 ) 3 dual-modified Na 2 Fe 0.6 Mn 0.4 PO 4 F composites were studied, and it was found that the capacity attenuation was due to irreversible structural changes such as agglomerated block cracking and structural collapse during multiple cycles, as well as the gradual thickening of the SEI film with the increase in cycle times. This study aims to apply N-RGO/Na 3 V 2 (PO 4 ) 3 dual-modified Na 2 Fe 0.6 Mn 0.4 PO 4 F composites to cathode materials for sodium-ion batteries, providing a theoretical basis for the development of fluorinated poly-anion compounds.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2011
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IF 4.746
Xiaolin Qiu,Wei Li,Guolin Song,Xiaodong Chu,Guoyi Tang
Microencapsulations of n-octadecane with different crosslinked methylmethacrylate-based polymer as shells were carried out by suspension-like polymerizations. 1,4-butylene glycol diacrylate (BDDA), divinylbenzene (DVB), trimethylolpropanetriacrylate (TMPTA) and pentaerythritol tetraacrylate (PETRA) were employed as crosslinking agents. The influences of the type and amount of crosslinking agent, the type of initiator and polymerization temperature on the properties of as-prepared microencapsulated phase change materials (MicroPCMs) have been studied. The MicroPCMs were characterized using Fourier transformed infrared (FTIR) spectroscopy and scanning electron microscopy (SEM). Thermal properties and thermal stability of MicroPCMs were investigated by differential scanning calorimetry (DSC) and thermalgravimetric analysis (TGA). Shell mechanical strength was measured by micro/nano-hardness tester. Thermal properties, thermal resistant temperatures as well as shell mechanical strength of MicroPCMs enhanced as the number of crosslinkable functional moieties of the crosslinking agents increased. The MicroPCMs containing 75.3 wt% n-octadecane obtained using PETRA as crosslinking agent has the highest latent heats of melting (156.4 J/g) and crystallization (182.8 J/g) and displays the highest thermal stability and shell mechanical strength. The MicroPCMs prepared with DVB shows a relatively higher shell mechanical strength and heat capacity compared with those prepared with BDDA. Both heat capacity and thermal stability of MicroPCMs prepared by combining 2,2 ′ -azobisisobutyronitrile (AIBN) and redox initiators at 45 °C were lower than that of MicroPCMs prepared with AIBN or benzoyl peroxide (BPO) at 85 °C. Hence, MicroPCMs with crosslinked methylmethacrylate-based polymer as shells, especially crosslinked polymer shells of higher crosslinking density , show a good potential as a solar-energy storage material.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
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IF 4.182
Miao Zhang,Ruijin Zheng,Ying Ma,Ruiping Chen,Xun Sun,Xuan Sun
Three 2D N-rich COFs linked by –C=N– bond, named COF-SDU1, COF-SDU2, COF-SDU3, have been synthesized via the Schiff-base condensation reaction . Tri-(4-formacylphenoxy)-1,3,5-triazine (TRIF) is employed as N-rich aldehyde building block, and p-phenylenediamine (PA), hydrazine hydrate, and terephthalic dihydrazide (TPDH) are as the amine building blocks, respectively, which results in high crystallinity, high BET surface area, and abundant N-atom sites for COF-SDU1, COF-SDU2, and COF-SDU3. COF-SDU1 exhibits large CO 2 uptake of 741 mg g −1 at 298 K under 45 bar, while COF-SDU2 is 484 mg g −1 and COF-SDU3 is only 331 mg g −1 , which are closely related to their specific surface area but irrespective of the absolute N-content. The result clearly reveals the impact of various factors, including N-content, BET surface area and pore size on CO 2 storage performance. It shows that N-content determines capacities at low pressure (<1 bar), BET surface area plays the decisive role under relative low pressure (<25 bar) and large pore size helps enhance the capacity under relative high pressure (>25 bar). Among all factors, BET surface area plays the crucial role in determining the high-pressure CO 2 storage capacity, which is well verified by theoretical modeling.
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Journal of Energy Storage
·
2024
·
IF 8.9
Yuhan Ji,Tong Wang,Xu Yao,Jingkui Gao,Yanting Chu,Jingwen Sun,Haitao Dong,Jingquan Sha
Hard carbon (HC) with larger interlayer spacing, lower operation potential and stable skeleton is a promising kind of anode materials for sodium-ion batteries (SIBs), where heteroatom doping and structural design have been proved to be effective strategies to improve its Na + storage performance. Herein, biomass agar-derived N-doped porous carbon (NPC-Ts, T = 750, 900 and 1050 °C) were successfully fabricated by modulating carbonization temperature, where interlayer spacing, specifical surface area (SSA), micro/mesopore amount and N-doping levels and configurations (pyridinic N (N-6), pyrrolic N (N-5) and graphite N (N-Q)) were explored in detail. Among the NPC-900 shows the largest interlayer spacing (0.412 nm), SSA (3991 m 2 /g) and sum percentage of N-6 and N-5 (76.7 %). When applied as anode material for SIBs, NPC-900 exhibits the highly reversible capacity (430.9 mAh/g at 100 mA/g after 100 cycles) and excellent rate capability (162 mAh/g at 5000 mA/g) and outstanding cycle life (242.6 mAh/g at 1000 mA/g after 5000 cycles). More importantly, when coupled with Na 3 V 2 (PO 4 ) 3 (NVP) cathode, the Na + full cell displays the highest practical energy density of 267 Wh/kg to date, to the best our knowledge, revealing its potential practical sodium storage applications.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Tianle Liu,Shitian Zhao,Guokun Yang,Mingsheng Chen,Junhui Kou,Weijian Wang,Guosheng Jiang,Shaojun Zheng
Prominent thermal management, electromagnetic interference(EMI) shielding, and anti-ionizing radiation capabilities are essential trends in developing flexible materials. In this study, we developed a novel flexible MXene/polyvinyl alcohol/ microencapsulated phase change material (MPM) phase change composite film with a sandwich structure using an alternating vacuum filtration method. This film demonstrates good toughness, strength, stability, and durability. Incorporating microencapsulated phase change material(MEPCMs) enhances the enthalpy of the films (110.2J/g). Additionally, due to the incorporation of phase change microcapsules with a unique barium sulfate-based (BaSO 4 ) as the wall material, the films not only possess EMI shielding performance(39.7 dB), but also exhibits resistance to ionizing radiation(4.62 cm 2 g −1 ). Notably, the film can convert light and electrical energy into heat and store this heat as latent heat within the MEPCMs, enabling multi-source thermal management capability. The ease of preparation and exceptional performance of MPM make it highly suitable for a wide range of industrial and wearable applications.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-23
·
IF 14.7
Luo Yu-Wei,Zhou Jiang-Peng,Ji Hongyu,Xu Doudou,Zheng Anqi,Wang Xin,Dai Zhizheng,Luo Zhicheng,Cao Fang,Wang Xing-Yue,Bai Yunfang,Chen Di,Chen Yueming,Wang Qi,Yang Yaying,Zhang Xinghai,Chiu Sandra,Peng Xiaozhong,Huang Ai-Long,Tang Kai-Fu
Though RNAi and RNA-splicing machineries are involved in regulating severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) replication, their precise roles in coronavirus disease 2019 (COVID-19) pathogenesis remain unclear. Herein, we show that decreased RNAi component (Dicer and XPO5) and splicing factor (SRSF3 and hnRNPA3) expression correlate with increased COVID-19 severity. SARS-CoV-2 N protein induces the autophagic degradation of Dicer, XPO5, SRSF3, and hnRNPA3, inhibiting miRNA biogenesis and RNA splicing and triggering DNA damage, proteotoxic stress, and pneumonia. Dicer, XPO5, SRSF3, and hnRNPA3 knockdown increases, while their overexpression decreases, N protein-induced pneumonia’s severity. Older mice show lower expression of Dicer, XPO5, SRSF3, and hnRNPA3 in their lung tissues and exhibit more severe N protein-induced pneumonia than younger mice. PJ34, a poly(ADP-ribose) polymerase inhibitor, or anastrozole, an aromatase inhibitor, ameliorates N protein- or SARS-CoV-2-induced pneumonia by restoring Dicer, XPO5, SRSF3, and hnRNPA3 expression. These findings will aid in developing improved treatments for SARS-CoV-2-associated pneumonia.
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yuqing Dong,Chengsen Li,Shuting Zhang,Xiangwei Meng,Meijie Yu
Prussian blue (PB) as a type of metal-organic framework has attracted widespread attention in the field of electromagnetic wave (EMW) absorption due to its adjustable composition and structure. N-doped porous carbon/rGO/Fe 4 N composite is prepared by carbonizing and nitriding PB precursor. Fe 4 N/rGO/NPC exhibits the minimum reflection loss (RL min ) is −53.09 dB at 16.16 GHz of 2.2 mm, with an effective absorption bandwidth (EAB) value of 7.84 GHz (10.16–18 GHz) at 2.6 mm. The EMW absorption mechanisms analysis displayed that excellent impedance matching and various attenuation pathways including magnetic loss, conduction loss, interfacial and dipole polarization synergistically contributed to the high EMW absorption performances. The results indicate that the Fe 4 N/rGO/NPC composite derived from PB precursor presents great potential in the field of EMW absorption.
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CATALYSIS SURVEYS FROM ASIA
·
2025
·
IF 2.3
Zhu Mengxuan,Li Hongqing,Wang Xin,Wang Longyang,Wang Rui,Jiang Heng,Jin Changzi
Design of efficient metal-acid bifunction catalysts is of significance for development of hydroisomerization of linear alkanes. In this study, the spatial configurational construction of Pt-ZSM-5 catalytic system was achieved by fabrication of acidic ZSM-5 zeolite and mesoporous silica core-shell composites equipped with controlled location of Pt sites, which aim to explore the effect of functional sites proximity on isomerization reactivity. A series of characterization techniques such as X-ray diffraction, transmission electronic microscopy, N 2 physical adsorption, NH 3 temperature programmed desorption, X-ray photoelectron spectroscopy and so on had confirmed that the synthesized core-shell bifunctional catalysts with different Pt location possessing similar textural, acid and metal properties. In the catalytic hydroisomerization of n -heptane, however, the catalyst with Pt sites locating at acid zeolite exhibits superior n -heptane conversion and isomerization selectivity, which indicates that proximity of active sites at atomic scale may be more conducive to their synergistic effect when the diffusional limitation from zeolitic channel is minimized. These results had presented new direction for the preparation of efficient bifunctional catalysts in hydroisomerization of linear alkanes.
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Nanoscale
·
2024
·Vol. 16
·期 10
·5215-5221
·
IF 5.8
Yangdong Zhou,Junda Chen,Zhiyin Huang,Yuqin Peng,Lixin Xing,Chunmei Tang,Ning Wang,Ling Meng,Mingjie Wu,Lei Du,Siyu Ye
The cathodic oxygen reduction reaction (ORR) has been continuously attracting worldwide interest due to the increasing popularity of proton exchange membrane (PEM) fuel cells. So far, various Pt-group metal (PGM) or PGM-free catalysts have been developed to facilitate the ORR. However, there is still a gap to achieve the expected goals as proposed by the U.S. Department of Energy (DoE). Recently, PGM-free@PGM hybrid catalysts, such as the M/N/C@PtM catalyst, have achieved the milestones of oxygen reduction, as reviewed in our recent work. It is, nevertheless, still challenging to unravel the underlying structure–property relationships. Here, by applying different Pt/Co ratios, a series of Co/N/C@PtxCo catalysts are synthesized. Interestingly, the ORR activity and stability are not linear with the Pt content, but show a volcano-like curve with increased Pt usage. This relationship has been deeply unraveled to be closely related to the contents of pyrrolic N, pyridinic N, and graphitized carbon in catalysts. This work provides guidelines to rationally design the coupled PGM-free@PGM catalysts toward the ORR by appropriate surface engineering.
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