Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Guo Qiubo,Han Shuai,Lu Yaxiang,Xiao Ruijuan,Li Jin,Hao Qingli,Rong Xiaohui,Weng Suting,Niu Yaoshen,Ding Feixiang,Yang Yang,Xia Hui,Wang Xuefeng,Xie Fei,Zhou Lin,Hou Xueyan,Li Hong,Huang Xuejie,Chen Liquan,Hu Yong-Sheng
Prussian blue analogues (PBAs) are promising electrode candidates for aqueous batteries because the inevitable interstitial water is generally thought to have little impact on battery performance. Currently, mounting researches have focused on optimizing PBA properties by varying transition metal composition, but less attention has been paid to interstitial water, especially in alkali metal-ion deficient PBAs with large cavities. Here, we employ the water-rich K 0.01 Mn[Cr(CN) 6 ] 0.74 ·4.75H 2 O as the negative electrode to study the effect of interstitial water. It is found that during de-potassiation, the electrode undergoes dehydration, which negatively impacts kinetics, distorts structure, and raises charging potential. A cation-self-shielding strategy involving Dihydroxyacetone (DHA) in the electrolyte to secure the water-rich state is then proposed. The built 1.82 V all-Prussian blue aqueous K-ion battery delivers a high practical specific energy of ~76 Wh kg −1 over 1.5 V (based on the total mass of active materials in both electrodes). This study reveals the significance of interstitial water on the kinetics of PBA negative electrodes and promotes the exploration of water-containing electrodes to develop high-voltage aqueous rechargeable batteries for energy storage applications.
研究领域:
储能
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材料科学
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电化学
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电池技术
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DOI
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Danli Tang,Dengjie Zhong,Yongxian Zhou,Yunlan Xu,Tanxia Xiang,Wantao Li,Yuanfang Yang,Chunmiao Fan,Jisai Chen
In this study, the magnetic composite catalyst, CuFe2O4 modified Co-Al layered double hydroxide supported by alkali-activated N,S-codoped biochar (CFO/CoAl-LDH@K-NSBC) was developed to activate ozone to degrade methylene blue (MB). The MB degradation efficiency of the CFO/CoAl-LDH@K-NSBC/O3 system was 96.30% in 7 min, and it still remained at 92.85% after 5 cycles. Notably, in the pond water matrix, the degradation efficiency only decreased by 6.44% after five cycles, which confirmed its remarkable stability and application prospects. Electrochemical analysis revealed that the comodification of CFO and CoAl-LDH significantly enhanced the charge transfer and catalytic activity of K-NSBC. The results of material characterization and quenching experiments showed that highly exposed active sites, including oxygen vacancies (Ov), Co3+/Co2+, Fe3+/Fe2+, Cu2+/Cu+, pyridinic N, graphitic N and thiophenic S, synergistically drove O3 activation to generate 1O2, ·OH, and ·O2– to participate in MB degradation, among which 1O2 was the main reactive oxygen species. This study provides a novel approach for the preparation of environmentally friendly biochar-based multimetal oxides with high catalytic activity.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jianghua Wu,Faisal Faiz,Mashkoor Ahmad,Miao Zhengjie,Zha Qiang,Wei Xu,Xiaojin Zhao,Xiaofang Pan,Yasir Faiz
The fabrication of supercapacitors with outstanding performance is presented with a distinct defect-rich nanostructures. A one-pot, energy-efficient method for synthesizing defective manganese dioxide nanowires doped with potassium (K 0.35 MnO 2 ) was developed. The introduction of potassium ions at 35 % birnessite resulted in a significant increase in lattice defects and an improvement in conductivity. Addition of KOH induces a phase transition from α-MnO 2 to δ-MnO 2 . These imperfections result in a greater quantity of active sites, which are crucial for the process of energy storage. The K 0.35 MnO 2 structure demonstrates a 405F/g increased capacity at a current density of 1 A/g. The asymmetric supercapacitor (K 0.35 MnO 2 /AC) that was manufactured exhibits a capacitance of 106.4F/g when operating at 1 A/g, while maintaining a maximum energy density of 71.5 Wh kg −1 and a power density of 672 W kg −1 . Furthermore, 92.7 % of the initial capacitance of the device is retained even after 8,000 cycles at 20 A/g. This study presents novel insights into the production of defective materials for energy storage applications through the utilization of a one-pot process as opposed to the multi-step method. In order to produce high-performance supercapacitors for practical applications, the results indicate that defect engineering is a crucial factor.
研究领域:
材料科学
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电化学
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DOI
高影响因子
DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 41
·18012-18018
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IF 4.197
Yongfeng Liu,Yaxiong Yang,Xin Zhang,You Li,Mingxia Gao,Hongge Pan
The thermal dehydrogenation process of the KOH-containing Mg(NH2)2–2LiH system was systematically investigated by identifying changes in the structure and composition of its components by XRD and FTIR. During ball milling, the added KOH reacts with Mg(NH2)2 and LiH to produce MgO, KH and Li2K(NH2)3. During the initial heating process (<120 °C), the newly formed KH and Li2K(NH2)3 react with Mg(NH2)2 and LiH to yield MgNH, LiNH2 and Li3K(NH2)4 along with hydrogen release. Raising the temperature to 185 °C results in a reaction between Mg(NH2)2, MgNH and LiH that gives Li2Mg2N3H3 as the product and further releases hydrogen. As the temperature is increased to 220 °C, Li2Mg2N3H3 reacts with LiNH2 and LiH to produce Li2MgN2H2 and H2. Meanwhile, two parallel reactions between Li2Mg2N3H3, Li3K(NH2)4 and LiH also generate additional hydrogen. Specifically, the KH and Li2K(NH2)3, formed in situ during ball milling, serve as reactants in the dehydrogenation reaction of the Mg(NH2)2–2LiH system, which is responsible for the significantly improved thermodynamics and kinetics of hydrogen storage.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Fang Wang,Xueyan Wu,Yuxuan Han,Yan Lv,Jixi Guo,Xiaoman Li,Yaping Zhang
In cement kiln flue gas emissions, high concentrations of alkali and alkaline earth metals cause the deactivation of the NbCe/Ti catalysts, significantly reducing their operational lifespan under industrial conditions. Here, the NbCe-loaded titanium nanotubes (NbCe/TiNTs) catalyst has been synthesized via hydrothermal and impregnation methods. The NbCe/TiNTs catalyst exhibits superior resistance to potassium (K) and calcium (Ca) poisoning. Notably, NbCe/TiNTs catalyst maintains high NOx conversion across a wide temperature range (192–350 °C). The 5Ca-NbCe/TiNTs and 3K-NbCe/TiNTs catalysts achieve a 90% NOx conversion at 235 and 242 °C, respectively, demonstrating remarkable resistance to K and Ca poisoning. The results indicate that TiNTs supports enhance both the specific surface area and surface acid sites of the catalyst, synergistically improving its resistance to K and Ca poisoning. Furthermore, an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study elucidates selective catalytic reduction with the NH3 (NH3-SCR) reaction mechanism, revealing dual contributions from both the Eley–Rideal (E–R) and Langmuir–Hinshelwood (L–H) mechanisms on the catalyst. This work provides a research direction for enhancing the alkali poisoning resistance of NOx removal catalysts.
研究领域:
环境催化
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材料科学
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化学工程
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表面科学
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DOI
高影响因子
Chemistry-Switzerland
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2025
·Vol. 7
·期 5
·150
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IF 2.4
Ting Geng,Yuhan Qin,Zhuo Chen,Yuhan Sun,Ao Zhang,Mengyuan Lu,Mengzhen Lu,Siying Zhou,Yongguang Li,Guanjun Xiao
Lead-free perovskite variants have emerged as promising candidates due to their self-trapped exciton emission. However, in ASnX3systems, facile oxidation of Sn(II) to Sn(IV) yields A2SnCl6vacancy-ordered derivatives. Paradoxically, despite possessing a direct bandgap, these variants exhibit diminished photoluminescence (PL). Doping engineering thus becomes essential for precise optical tailoring of A2SnX6materials. Herein, through integrated first-principles calculations and spectroscopic analysis, we elucidate the luminescence mechanism in Te4+-doped (NH4)2SnCl6lead-free perovskites. Density functional theory, X-ray diffraction (XRD) patterns and X-ray photoelectron spectroscopy (XPS) confirm Te4+substitution at Sn sites via favorable chemical potentials. Spectral interrogations, including absorption and emission profiles, reveal that the intense emission originates from the triplet STE recombination (3P1→1S0) of Te centers. Temperature-dependent PL spectra further demonstrate strong electron–phonon coupling that induces symmetry-breaking distortions to stabilize STEs. Complementary electronic band structure and molecular orbital calculations unveil the underlying photophysical pathway. Leveraging these distinct thermal responses of PL intensity and peak position, 0.5%Te:(NH4)2SnCl6emerges as a highly promising candidate for non-contact, dual-parameter optical thermometry over an ultra-broad range (100–400 K). This work provides fundamental insights into the exciton dynamics and thermal engineering of optical properties in this material system, establishing its significant potential for advanced temperature-sensing applications.
研究领域:
材料科学
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凝聚态物理
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光学工程
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无机化学
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功能材料
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产品关联
DOI
高影响因子
Small
·
2025
·
IF 12.1
Qiankun Zhang,Zhewen Ma,Haimin Zhang,Xuan Lan,Zongkun Bian,Yongchun Luo
This study puts forward an innovative electrolyte design to resolve the problems of scarce efficient proton sources and interface instability in proton batteries. It verifies that hydrogen protons mainly come from water molecule dissociation, with acetic acid acting as an auxiliary source, leading to proton source concentration changes during charging/discharging. To address this, an ionic liquid (1-Ethyl-3-methylimidazolium acetate, abbreviated as [emim][Ac]) electrolyte containing acetic acid (HAc) and potassium acetate (KAc) ([emim][Ac] + 4 m HAc + 1 m KAc) is developed. Experimental results show the battery performs excellently, with a discharge capacity up to 1584 mAh g −1 , and retains 1217 mAh g −1 at a 6000 mA g −1 discharge current density after 300 cycles. Both experiments and simulations confirm H⁺ primarily comes from HAc and H 2 O solvated by K⁺ and imidazolium cations. K⁺ introduces a new “vehicle transport channel” to reduce proton transport resistance, while HAc and KAc form a buffer solution to optimize solvation structure and inhibit side reactions. Ionic liquids provide a stable environment for ion transport. This work offers references for developing high-rate, long-cycle proton batteries.
研究领域:
储能
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电化学
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材料科学
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化学工程
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电源技术
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Zhang Shi-Nan,Gao Peng,Liu Qian-Yu,Zhang Zhao,Leng Bing-Liang,Chen Jie-Sheng,Li Xin-Hao
Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particularly in pure nitrate solutions. Herein, we present the application of electron deficiency of Ru metals to boost the repelling effect of counter K + ions via the electric-field-dependent synergy of interfacial water and cations, and thus largely promote nitrate reduction reaction with a high yield and well-maintained Faradaic efficiency under ampere-level current density. The pronounced electron deficiency of Ru metals boosts the repelling effect on hydrated K + ions, as indicated by the distance of K + ions to catalyst surface, which can loosen the water layer to depress hydrogen evolution and accelerate nitrate conversion. Consequently, the optimized electrode loaded with electron-deficient Ru atomic layers can directly produce 0.26 M ammonia solution in pure nitrate solution in 6 h, providing a high yield (74.8 mg mg cat –1 h –1 ) and well-maintained the Faradaic efficiency for over 120 h under ampere-level reduction.
研究领域:
电化学
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催化材料科学
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DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Donglin,Sha Juncheng,Mei Xudong,Ye An,Zhao Zhengping,Qiu Xunlin,Liu Xiaoyun,Niu Yueping,Zuo Peiyuan,Zhuang Qixin
As integrated circuits have developed towards the direction of complexity and miniaturization, there is an urgent need for low dielectric constant materials to effectively realize high-fidelity signal transmission. However, there remains a challenge to achieve ultralow dielectric constant and ultralow dielectric loss over a wide temperature range, not to mention having excellent thermal conductivity and processability concurrently. We herein prepare dual-linker freestanding covalent organic framework films with tailorable fluorine content via interfacial polymerization. The covalent organic framework possesses an ultralow dielectric constant (1.25 at 1 kHz, ≈1.2 at 6 G band), ultralow dielectric loss (0.0015 at 1 kHz) with a thermal conductivity of 0.48 Wm −1 K −1 . We show high-fidelity signal transmission based on the large-sized (>15 cm 2 ) COF films, far exceeding the most commercially available polyimide-based printed circuit board. In addition, the covalent organic framework also features excellent electret properties, which allows for active high-temperature electromechanical sensing. The electrode nanogenerator maintains 90% of the output voltage at 120 °C, outperforming the traditional fluorinated ethylene propylene electret. Collectively, this work paves the way for scalable application of ultralow dielectric constant covalent organic framework thin films in signal transmission and electromechanical sensing.
研究领域:
材料科学
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电子工程
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纳米技术
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DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Wang Zhitong,Liu Dongyu,Xia Chenfeng,Shi Xiaodong,Zhou Yansong,Liu Qiuwen,Huang Jiangtao,Wu Haiyan,Zhu Deyu,Zhang Shuyu,Li Jing,Deng Peilin,Vasenko Andrey S.,Xia Bao Yu,Tian Xinlong
Acidic electrochemical CO 2 conversion is a promising alternative to overcome the low CO 2 utilization. However, over-reliance on highly concentrated K + to inhibit the hydrogen evolution reaction also causes (bi)carbonate precipitation to interfere with catalytic performance. In this work, under the screening and guidance of computational simulations, we present a carbon coated tip-like In 2 O 3 electrocatalyst for stable and efficient acidic CO 2 conversion to synthesize formic acid (HCOOH) with low K + concentration. The carbon layer protects the oxidized In species with higher intrinsic activity from reductive corrosion, and also peripherally formulates a tip-induced electric field to regulate the adverse H + attraction and desirable K + enrichment. In an acidic electrolyte at pH 0.94, only 0.1 M low K + is required to achieve a Faradaic efficiency (FE) of 98.9% at 300 mA cm −2 for HCOOH and a long-time stability of over100 h. By up-scaling the electrode into a 25 cm 2 electrolyzer setup, a total current of 7 A is recorded to sustain a durable HCOOH production of 291.6 mmol L −1 h −1 .
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
RARE METALS
·
2025
·
IF 11
Long Xia,Liu Xiao-Chi,Yang Yan-Yi,Dai Jia-Qing,Cao Jue-Xian,Hu Yong
Gaining insights into charge transport related to conformational changes and ion transport in valinomycin (VM) is crucial for understanding the underlying physiological processes and advancing ion carrier applications. Observing these processes in single molecules provides deeper insights and precision than those obtained through conventional ensemble measurements. Herein, we employed a single-molecule conductance measurement method based on the scanning tunneling microscopy break-junction (STM-BJ) to measure the charge transport of individual VM molecules in both non-polar and polar solvents, as well as when mediated by K + ions. Single-molecule conductance measurements revealed that the bracelet and propeller-type conformations of VM in both non-polar and polar solvents significantly affect its conductance. In polar solvents, the propeller-type conformation of VM demonstrated a well-defined conductance signature, single-molecule rectification feature, and through-space transmission mechanism. Specifically, the introduction of K + ions in polar solvents induced a conformational transition from the propeller-type to the bracelet-type form, facilitating K + binding recognition. These observations were further supported by density functional theory combined with non-equilibrium Green’s function calculations. This study enhanced the fundamental understanding of the electronic transport mechanisms in VM and valinomycin-K + molecular junctions, offering insights into VM ionophores and promoting supramolecular sensing applications. Graphical abstract
研究领域:
生物物理学
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纳米科技
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理论化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Li Gao,Tenghong Kong,Yanqing Ye,Peng Ren,Qiang Zhou,Huaijun Tang,Zhengliang Wang
Red-emitting Mn 4+ -doped fluoride phosphors are recognized as promising materials for high-performance warm white light-emitting diodes (WLEDs). However, the extensive use of toxic hydrofluoric acid in traditional synthesis methods hinders their development and commercialization. Furthermore, the traditional solid-phase method often has cumbersome sintering steps, high temperature, long holding time, and certain safety hazards, so it is very necessary to develop a green synthesis method with simple steps and low energy consumption. In this study, a low-temperature solid-state method is proposed to synthesize Rb A SiF 6 :Mn 4+ ( A = K, Cs) phosphors by one step. Optimal emission intensities were observed at Mn 4+ concentrations of 1.2 % in RbKSiF 6 and 2.1 % in RbCsSiF 6 . These phosphors demonstrated high thermal stability. At 423 K, the photoluminescence intensities of RbKSiF 6 :1.2 %Mn 4+ and RbCsSiF 6 :2.1 %Mn 4+ reached 114 % and 87 % of their respective values at room temperature. Meanwhile, the chromaticity shifts were almost negligible, and high color purity was achieved for both phosphors. The electro-optical performance of WLED devices utilizing these phosphors, in combination with YAG:Ce 3+ and GaN chips, showed high color rendering indices (CRI) and low correlated color temperatures (CCT) across varying currents. Specifically, under a driving current of 20 mA, the device incorporating RbKSiF 6 :1.2 %Mn 4+ exhibited a CRI of 94 and a CCT of 3732 K, with a luminous efficacy of 61 lm/W. These findings highlight the potential of green-synthesized RASFM phosphors in advancing the application of warm WLEDs.
研究领域:
材料科学
·
光学工程
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高影响因子
危险品化学品经营许可证（带存储）