APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Wei Li,Fei Wang,Xiao-shan Chu,Xiao-yun Liu,Yan-yan Dang
Water splitting by photocatalysis technique is regarded as an eco-friendly hydrogen production strategy. However, the poor photoresponsivity and automatic electron-hole recombination greatly restrict the HER performance of conventional semiconductor photocatalyst. Here, to utilize the stable electrochemical property of hexagonal phase boron nitride (h-BN) and improve its defect of wide bandgap ( E g ≈ 4.2 eV), reduced graphene oxide (rGO) was applied to construct three-dimensional (3D) porous h-BN/rGO hybrid accompanied by a carbon-doping strategy without template assistance, then a carbon-doped 3D porous h-BN/rGO (C-BNRG) hybrid with large BET surface area was successfully prepared. As the synergistic effect of h-BN/rGO heterointerface and carbon-doping, the improved photoresponsivity and electrochemical property were presented, and the resultant 3D porous C 0.4 -BNRG hybrid presented not only greatly enhanced HER activity (157.63 μmol·g −1 ·h −1 ) but excellent durability in pH = 8.5, which was prominently higher than pristine h-BN (~36.7 times), C-BN (~12.1 times) and 3D porous BNRG hybrid (~7.0 times). This study offers a template-free approach to develop non-metallic based 3D porous hybrid for outstanding HER performance.
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JOURNAL OF POWER SOURCES
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2024
·
IF 8.1
Zixuan Li,Dequan Bao,Wei Zhao,Wenxuan Xu,Yingheng Huang,Xiyong Chen,Hao Zhang,Xuhui Sun
Gel polymer electrolytes (GPEs) have emerged as a highly promising alternative to conventional liquid electrolytes for stable lithium-metal batteries (LIBs). However, their inherent poor mechanical properties and limited interfacial compatibility with lithium metal usually lead to unexpected growth of lithium dendrites , hindering commercial viability. Herein, an asymmetric polymer electrolyte with h-BN (HGPE) as protective layer was fabricated via a facile one-step coating strategy. Compared to pure GPE, the asymmetric polymer electrolytes exhibit significantly enhanced mechanical strength from 4.4 MPa to 7.4 MPa, effectively suppressing lithium dendrite growth. Furthermore, the HGPE improves interfacial compatibility with the anodes by preventing direct contact between GPE and lithium metals. The addition of h-BN also enhances the lithium-ion transfer number (t Li+ ), reaching 0.87 compared to 0.53 for pure GPE, attributed to the hindrance of anion movement by the protective layer. Consequently, the Li symmetric battery assembled with HGPE demonstrate exceptional long-term stability, maintaining performance over 1600 h at 0.1 mA cm −2 . Furthermore, the assembled Li|LiFePO 4 battery can deliver a high-capacity retention rate of 93.8 % after 500 cycles at room temperature, showcasing the promising potential of asymmetric polymer electrolytes for high-performance LMBs.
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Scientific Reports
·
2022
·Vol. 12
·期 1
·1-12
·
IF 4.996
Zhu Xinhe,Fu Jingguo,Ma Dengqing,Ma Chunsheng,Fu Yunyang,Zhang Zhuokai
A composite ceramic coating containing h-BN particles was prepared on the ZL109 alloy via plasma electrolytic oxidation. The h-BN particles were modified by Polyethylene glycol to improve the dispersibility. The results revealed that the h-BN particles in the electrolyte were inertly incorporated into the coating. Meanwhile, the incorporation of h-BN particles can reduce the porosity and slightly increase the roughness of the composite ceramic coating. Furthermore, the growth rate of the coating and the conversion of γ-Al 2 O 3 and α-Al 2 O 3 were promoted by the incorporation of h-BN particles via the change of the current. In addition, due to the presence of h-BN particles, the composite ceramic coating had a lower friction coefficient and a lower wear rate under dry sliding condition.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Kezhu Xu,Jin Wu,Qunling Fang,Linfeng Bai,Jinyu Duan,Jiaxing Li,Huajian Xu,Ailing Hui,Lingyun Hao,Shouhu Xuan
The organic pollutants and heavy metal ions are critical harmful substances in waste water because they destroy the ecological systems and lead diseases to animals and human beings. Unfortunately, the simultaneously remove of them in one system is still a challenge due to their different treating mechanism. Herein, a novel magnetic h-Fe 3 O 4 @Au/Polydopamine (Au/PDA) hybrid hollow nanosphere which can both absorb the potentially toxic U(VI) ions and catalyze the reduction of the 4-nitrophenol is reported. By using a simple in situ redox-oxidizing polymerization method, the h-Fe 3 O 4 hollow nanosphere is well encapsulated by the Au/PDA hybrid shell to form the dual-functional magnetic hollow nanocomposites. Owing to the hollow interior, uniform and functional PDA coating, and high active Au nanocrystals, the final h-Fe 3 O 4 @Au/PDA hollow nanosphere possesses high potential in nanocatalysis, heavy metal ions adsorption, and drug delivery. Because of the PDA protection, the h-Fe 3 O 4 @Au/PDA nanosphere can even keep 90% activity after 7 cycling catalytic reactions on reduction of 4-nitrophenol. Similarly, the h-Fe 3 O 4 @Au/PDA exhibits a good adsorption effect for U(VI) in nuclear waste and its adsorption capability reaches to 82.9 mg·g −1 by 6 successive adsorption–desorption experiments. Due to the facile magnetic separation, the h-Fe 3 O 4 @Au/PDA nanosphere can be easily collected by applying an external magnetic field. In summary, such a multifunctional recyclable h-Fe 3 O 4 @Au/PDA nanosphere with green and facile synthesis, easy manipulation, efficient adsorption performance and good catalytic activity possesses broad application potential in treatment of coexisting toxic water pollution.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengting Liu,Fu Yang,Hongyao Zhao,Xiu Zhong,Ruiting Ni,Kwame Nana Opoku,Zhenxiao Wang,Yangping Zhang,Yanyun Wang,Feng Zeng,Yinlong Zhu,Weidong Shi
In electrochemical nitrate reduction reaction (NITRR), the generation of active hydrogen (*H) and its poor utilization in conversion of various nitrate intermediates often cause mismatched kinetics, resulting in low ammonia yield rate (YR NH3 ) and Faraday efficiency (FE NH3 ). Herein, we construct a spatially-confined Cu/Fe 2 O 3 heterointerfaces within porous carbon fiber, featuring oxygen vacancy-rich iron oxide nanoparticles (∼14.7 nm) interface-coupled well-dispersed Cu nanocrystals. The interfacial metallic copper sites with optimized interfacial electron transfer accelerate the consumption of NO 2 – through supplying the most abundant active *H to equilibrate NITRR kinetics. The easy desorption of generated NH 3 from active sites facilitates the accelerated reaction cycles by rapidly exposing the spent active sites. Correspondingly, this catalyst achieves nearly 100 % nitrate conversion, with a YR NH3 of 81.3 mg h −1 mg cat -1 , FE NH3 of 98.11 %, and 100 % NH 3 selectivity without any nitrite accumulation, outperforming most state-to-art catalysts as reported. Impressively, when nitrite acts as reactant, ammonia synthesis through nitrite reduction reaches YR NH3 of 99 mg h −1 mg cat -1 and FE NH3 of 99.44 % outperforming all the same series reported. Moreover, active *H quenching and isotope labeling experiments uncover the generation of the most abundant active *H species and their high utilization among the reported results. Density function theory (DFT) calculations further indicate the interfacial Cu/Fe 2 O 3 regulates the d-band center of the catalyst, optimizing the adsorption of nitrate and further lowering the reaction energy barrier of the decisive step (*NO→*NOH).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xinru Wang,Yannan Zhou,Jiaoyu Peng,Wenhu Li,Xin Liu
Octadecylamine hydrochloride (ODA H) as an efficient flotation collector is extensively employed in KCl manufacturing. However, the residual of ODA-H not only directly influences KCl application fields, but also poses environmental risks owing to its low biodegradability. Meanwhile, the removal cost is comparatively high because of KCl solubility. In this study, a simple yet effective strategy was proposed to achieve efficient in-situ desorption of ODA-H from the solid KCl surface. The desorption behavior and underlying mechanism were systematically investigated, focusing on charge state conversion, interfacial wettability change, and ODA-H aggregation. The results demonstrated that OH − significantly enhanced the removal efficiency of ODA H, with a removal rate of 86 % achieved when the pH of the saturated KCl solution was raised to 14. In-situ Raman spectroscopy and Molecular Dynamics simulation elucidated the mechanism of OH − , which could accelerate ODA-H desorption kinetics by disrupting the electrostatic interaction between ODA-H and KCl surface, thereby altering its aggregation behavior. Furthermore, the disruption mechanism of interfacial hydrogen-bonding networks during the OH − -promoted desorption process was confirmed. The synergistic effects resulting from these enhancements facilitated the highly efficient desorption of ODA-H from the solid KCl surface. Importantly, industrial-grade KCl was refined with the ODA-H desorption efficiency of 73.95 %. This study will provide a new idea and mechanism explanation for the removal of pollutants on the soluble solid surface in high-salt solution.
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高影响因子
CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Xin Liu,Dining Li,Hui Xie,Jiachen Yao,Xuyan Shen,Haochuan Wang,Zhengyao Qu,Zuhua Zhang,Pan Feng
Alkali-free aluminum sulfate (AS)-based accelerators have become a widely adopted and indispensable admixture for shotcrete applications. However, their effects on the formation kinetics and properties of calcium silicate hydrate (C-S-H) – the primary hydrate in shotcrete – remain insufficiently understood. To bridge this knowledge gap, a combination of isothermal calorimetry, QXRD, and TGA was employed to uncover the temporal evolution of C-S-H. In addition, the chemical compositions and silicate chain structure were comprehensively examined using BSE-EDS, 27 Al NMR, coupled with 29 Si NMR techniques. Our results demonstrate that AS addition accelerated C 3 S hydration, promoting the C-S-H nucleation and growth rate. This acceleration effect can be ascribed to (1) the accelerated dissolution of silicate phases at early stages, and (2) the formation of divergent C-S-H needles, providing more nucleation sites while mitigating impingement between adjacent C-(A)-S-H needles. Multiple characterizations confirmed the enhanced incorporation of aluminum into C-S-H, predominately at the bridging site. Notably, increasing AS content decreased the Si/Ca of the C-(A)-S-H and concurrently enhanced the aluminum incorporation. This compositional shift led to the formation of longer aluminosilicate chains and concomitant improvements in the hardness and elastic modulus of C-(A)-S-H. These findings offer valuable insights into AS-induced alterations in C-(A)-S-H within accelerated cement pastes, facilitating the deeper understanding of the role of C-(A)-S-H in strength development and long-term durability of shotcrete.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shaohui Xiong,Xingyi Ou,Qingquan Liu,Yiwen Li,Juntao Tang,Guipeng Yu,Chunyue Pan,Shibo Guo,Sitong Li,Menghan Yong
Polymers of intrinsic microporosity (PIM) have attracted considerable attention in the development of mixed matrix membranes (MMMs) for CO 2 separation. A prominent challenge lies in engineering the spacing of the polymer matrix chains while eliminating non-selective interfacial defects. In this study, a CO 2 -philic triazine-based porous polymer, featuring robust hydrogen bond donating groups, was employed to fabricate a series of interfacial defect-free PIM-1 based MMMs (denoted as PIM-1/CSU-1). The interfacial adhesion and compatibility have been greatly improved due to the strengthened hydrogen bond interaction, which was systematically validated through variable-temperature infrared spectroscopy. Additionally, the formation of hydrogen bonds allowed for the regulation of the polymer matrix chain spacing, making the chain distance loose. Remarkably, the resulting membrane exhibited a CO 2 permeability of 13,429 Barrer and CO 2 /N 2 selectivity of 33.1—246.6% and 70.2% higher than pristine PIM-1, respectively, surpassing the latest Jansen/McKeown upper bound established in 2019, but also significantly exceed the performance of previously reported MMMs for CO 2 separation. The strategy of mitigating interfacial defects through the formation of hydrogen bonds between fillers and the polymer matrix emerges as a viable and effective method for fabricating gas separation membranes with exceptional separation capabilities.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Dong Anrui,Lin Gaoxin,Li Zhiheng,Wu Wen,Cao Xing,Li Wenlong,Wang Linqin,Zhao Yilong,Chen Dexin,Sun Licheng
The mechanical stability of the catalytic electrodes used for hydrogen evolution reactions (HER) is crucial for their industrial applications in anion exchange membrane water electrolysis (AEM-WE). This study develops a corrosion strategy to construct a self-supported electrocatalyst (Int-Ni/MoO 2 ) with high mechanical stability by anchoring the Ni/MoO 2 catalytic layer with a dense interlayer of MoO 2 nanoparticles. The Int-Ni/MoO 2 exhibits a strengthened homostructural interface between the interlayer and catalytic layer, preventing the detachment of the catalyst during ultrasonic treatment. The blade-shaped catalytic layer reduces bubble shock and potential fluctuations at high current densities up to −6000 mA cm −2 . As a result, the Int-Ni/MoO 2 electrode exhibits a low overpotential of 73.2 ± 14.2 mV and long-term stability for 6000 h at −1000 mA cm −2 in a 1 M KOH solution. The Int-Ni/MoO 2 assembled AEM-WE device demonstrates long-term stability at 1000 mA cm −2 for 1000 h with a very low degradation rate of 3.96 µV h −1 .
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PubMed
高影响因子
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
·
2015
·Vol. 2016
·期 2
·325-330
·
IF 3.065
Wannian Zhao,Lei Xu,Yingcai Ding,Ben Niu,Ping Xie,Zhaogang Bian,Denghong Zhang,Aihua Zhou
Coumarin derivatives are highly valuable compounds in drug discovery. Herein, we have developed two new coupling reactions that involve coumarins and either aldehydes or di- tert -butyl peroxide (DTBP) in the presence of inexpensive copper or iron catalysts. Both of these reactions proceed through a C(sp 2 )–H functionalization process to regioselectivity generate keto- or methyl-substituted coumarin derivatives in moderate to good yields These coupling reactions will enrich current coumarin chemistry. Graphical Two coupling reactions that regioselectively yield either keto- or methyl-substituted coumarin derivatives by proceeding through a C(sp 2 )–H functionalization process were successfully developed. The coupling of coumarins with either aldehydes or di- tert -butyl peroxide (DTBP) generated the corresponding products in moderate to good yields.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Chia-Tse Lee,Haoyuan Zheng,Chen Jin,Hang Che,Li Wang,Yuyuan Zhao,Shixuan He,Xinhua Wang,Yifeng Yu,Mi Yan
Metal nitrogen hydride (Li-Mg-N-H) is regarded as an ideal hydrogen storage material for automotive applications due to its advantages of high hydrogen storage capacity (5.6 wt%), low operating temperature, and good cycling performance, but the comprehensive hydrogen storage performance of this material still could be improved. For this reason, this paper constructed a Li-Na-Mg-N-H composite system by synthesizing NaMgH 3 to replace MgH 2 in the Li-Mg-N-H system. The improvement of the hydrogen absorption and desorption properties of the composite system after the replacement of MgH 2 by NaMgH 3 was investigated. Various properties and test results showed that the composite system after the replacement of MgH 2 by NaMgH 3 showed better hydrogen absorption and desorption properties. The initial/peak hydrogen release temperatures of Li-Na-Mg-N-H decreased from 135 ˚C/245 ˚C to 105 ˚C/145 ˚C, and the apparent activation energy of hydrogen release was reduced from 114.90 to 104.05 kJ/mol which means the kinetics of hydrogen absorption and desorption was greatly improved. The mechanism study shows that NaMgH 3 will react with LiNH 2 and forms the intermediate product Li 3 Na(NH 2 ) 4 during the hydrogen release process, which changes the hydrogen desorption pathway of the composite system and thus the hydrogen absorption and desorption kinetics were improved.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Mengfei Zhu,Yuepeng Pang,Fuqiang Lu,Xinxin Shi,Junhe Yang,Shiyou Zheng
Li–B–H complexes facilely prepared via partial dehydrogenation of LiBH4 are presented in this study as solid electrolytes for Li batteries. An exceptionally high Li-ion conductivity is found for the Li–B–H complex with 7.5 wt % H2 desorption under 3 bar H2 pressure, which reaches 2.7 × 10–4 S cm–1 at 35 °C, more than 4 orders higher than that of LiBH4. In-depth characterizations show that LiH and [Li2B12H11+1/n]n are in situ formed in the LiBH4 matrix and the interface layer between [Li2B12H11+1/n]n and LiBH4 is believed to be responsible for the high Li-ion conductivity. Moreover, this Li–B–H complex also exhibits excellent electrochemical stability, which enables the stable cycling of all-solid-state batteries at room temperature.
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