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学者姓名：龙金林
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Abstract ：
CH3OH is the most desired product of photocatalytic CH4 conversion. The prominent metal-decorated photocatalyst is challenging in both high yield and selectivity for CH3OH products due to over-oxidation by center dot OH mechanism. Here, interstitial Zn is fabricated into ZniO to induce the formation of Zn atom island for rapid single electron reduction of O2 into center dot OOH instead of center dot OH for the selective combination with methyl into CH3OOH. AuPd alloy is simultaneously decorated on ZniO surface for tuning CH3OOH adsorption and reduction into CH3OH. The synergy of Zn atom island and AuPd alloy achieve a tandem reaction pathway (CH4 -> CH3OOH -> CH3OH) for an unprecedented CH3OH yield of 2444 mmol gAuPd-1 h-1 (or 8800 mu mol gcat-1 h-1) with 98.3% selectivity, which bypasses the center dot OH mechanism for tuning the high selectivity of CH3OH. An apparent quantum efficiency of 18.53% at 370 nm for CH4 conversion are super to the reported photocatalytic systems. Thus, this work provides the new strategy of the synergetic atom island and metal alloy photocatalysts through a tandem reaction pathway to mediate the photocatalytic selective oxidation of CH4 into the desired CH3OH.
Keyword ：
atom island atom island AuPd alloy AuPd alloy methanol selectivity methanol selectivity photocatalysis photocatalysis tandem reaction tandem reaction
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| GB/T 7714 | Xiao, Zhen , Shen, Jinni , Jiang, Jianing et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Xiao, Zhen , Shen, Jinni , Jiang, Jianing , Zhang, Jiangjie , Liang, Shuqi , Han, Shitong et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni-1 SAC on beta-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni-1/beta-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni-1/beta-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
Keyword ：
biomass biomass carbide carbide catalysis catalysis hydrodeoxygenation hydrodeoxygenation single-atom catalyst single-atom catalyst
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| GB/T 7714 | Guo, Haoquan , Zhao, Jiwu , Chen, Yu et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C [J]. | ACS CATALYSIS , 2024 , 14 (2) : 703-717 . |
| MLA | Guo, Haoquan et al. "Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C" . | ACS CATALYSIS 14 . 2 (2024) : 703-717 . |
| APA | Guo, Haoquan , Zhao, Jiwu , Chen, Yu , Lu, Xinyu , Yang, Yue , Ding, Chenrong et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C . | ACS CATALYSIS , 2024 , 14 (2) , 703-717 . |
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Wound dressings play a critical role in the wound healing process; however, conventional dressings often address singular functions, lacking versatility in meeting diverse wound healing requirements. Herein, dual-network, multifunctional hydrogels (PSA/CS-GA) have been designed and synthesized through a one-pot approach. The in vitro and in vivo experiments demonstrate that the optimized hydrogels have exceptional antifouling properties, potent antibacterial effects and rapid hemostatic capabilities. Notably, in a full-thickness rat wound model, the hydrogel group displays a remarkable wound healing rate exceeding 95% on day 10, surpassing both the control group and the commercial 3M group. Furthermore, the hydrogels exert an anti-inflammatory effect by reducing inflammatory factors interleukin 6 (IL-6) and tumor necrosis factor-alpha (TNF-alpha), enhance the release of the vascular endothelial growth factor (VEGF) to promote blood vessel proliferation, and augment collagen deposition in the wound, thus effectively accelerating wound healing in vivo. These innovative hydrogels present a novel and highly effective approach to wound healing. Dual network multifunctional hydrogels are developed using a one-pot synthesis approach. The in vitro and in vivo experiments demonstrate that these hydrogels have exceptional antifouling properties, potent antibacterial effects and rapid hemostatic capabilities.
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| GB/T 7714 | Jiang, Hongzhi , Huang, Xueping , Yang, Jiachao et al. Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing [J]. | JOURNAL OF MATERIALS CHEMISTRY B , 2024 , 12 (20) : 4909-4921 . |
| MLA | Jiang, Hongzhi et al. "Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing" . | JOURNAL OF MATERIALS CHEMISTRY B 12 . 20 (2024) : 4909-4921 . |
| APA | Jiang, Hongzhi , Huang, Xueping , Yang, Jiachao , Yu, Xunbin , Yang, Weibo , Song, Yunhao et al. Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing . | JOURNAL OF MATERIALS CHEMISTRY B , 2024 , 12 (20) , 4909-4921 . |
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Aiming to improve the decay in thermochemical energy storage (TCES) performance of CaO-based looping materials with the number of carbonation/calcination cycles, a series of Y/Mg-codoped CaO-based materials were prepared by using the classical sol-gel method and citric acid as a carbon template to enhance the porosity and specific surface area. The structural characterizations showed that Y and Mg were presented in two forms. Part of Y/Mg was presented in the form of Y2O3 and MgO nanoparticles with an average size of 15 and 40 nm, respectively. These Y2O3 and MgO nanoparticles with high Tammann temperature and thermal conductivity were highly dispersed to retard the sintering and growth of CaO grains. The rest of Y and Mg were doped into the framework of the CaO lattice in atomic form by substituting Ca atoms. These Y and Mg created a large amount of the oxygen vacancies surrounding Ca atoms to facilitate the electron transfer from Ca2+ ions to dopants, which enhanced the CO2 capture capacity of CaO-based materials by improving the kinetics of the carbonation reaction. As a result, the optimal CaO-based composite denoted as Ca/Y5/Mg10 exhibited a high initial energy storage density of up to >2300 kJ/kg and held an excellent looping reaction stability after 25 carbonation/calcination cycles owing to the cooperation of Y with Mg additives. This work provided effective and economical CaO-based looping materials for application in thermochemical energy storage.
Keyword ：
CaO-based materials CaO-based materials carbonation/calcination cycles carbonation/calcination cycles sintering resistance sintering resistance thermochemical energy storage thermochemical energy storage Y/Mg codoping Y/Mg codoping
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| GB/T 7714 | Wang, Jifu , Xiong, Wei , Ding, Zhengxin et al. Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg [J]. | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (24) : 12165-12173 . |
| MLA | Wang, Jifu et al. "Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg" . | ACS APPLIED ENERGY MATERIALS 7 . 24 (2024) : 12165-12173 . |
| APA | Wang, Jifu , Xiong, Wei , Ding, Zhengxin , Wang, Pengzhao , Long, Jinlin . Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg . | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (24) , 12165-12173 . |
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光催化水分解制氢是解决环境污染和能源危机的理想途径.共价有机骨架(COFs)作为一类由共价键连接的周期性网状拓扑材料,其电子结构和化学性质可在分子水平上进行定制和调控,是研究半导体光催化剂构-效关系的理想模型.为了提高COFs的电荷分离效率,在COFs骨架上设计供体-受体(D-A)单元,构筑分子内电场(IMEF)促进电荷定向迁移是一种行之有效的策略.然而,在亚胺键连接的COFs中,亚胺键取向诱导产生的键内电场(IBEF)对光生激子的分离效率的影响往往被忽视.因此,进一步研究IMEF与IBEF之间的相互作用对COFs内光生电子转移动力学的影响具有重要意义,可为深入揭示光催化产氢机制提供关键信息. 本文报道了一种基于COFs的双电场叠加策略,用于提高光催化产氢反应效率.首先,通过将有机单元的末端官能团进行互换,利用水热法成功制备了两种亚胺键取向相反的强D-A型COFs光催化剂,TNCA和TCNA.其中,官能团的微小变化保证了由D-A结构组成的IMEF方向和强度的一致性,可以使得在仅改变IBEF的情况下全面研究COFs的电子结构.X射线粉末衍射、傅里叶变换红外光谱、固体核磁以及X射线光电子能谱等结果证实了两种COFs的成功合成.随后,扫描电镜、透射电镜和氮气等温吸脱附曲线结果表明两种COFs均为介孔材料.紫外-可见漫反射光谱结果表明,所制备的催化剂具有良好的可见光吸收能力,结合莫特肖特基曲线结果,表明催化剂在热力学上均满足光催化产氢的要求.采用光致发光光谱、时间分辨荧光光谱、电子顺磁共振、光电流以及电化学阻抗研究了两种催化剂的载流子分离和转移行为,并且利用飞秒瞬态吸收光谱进一步明确了COFs中光生电荷转移动力学过程.结果表明,相较于TCNA,TNCA在光照下能够产生更多的光生电子且具有更长的寿命.光催化产氢活性评价结果显示,在可见光(A ≥ 420nm)照射下,具有同向叠加电场的TNCA,光催化析氢速率高达57.3 mmol·g-1·h-1,是具有相反电场取向TCNA(0.11 mmol·g-1·h-1)的520倍.并且TNCA具有更负的导带能级,有利于光生电子参与还原过程,最终获得较好的光催化析氢性能.此外,理论计算结果表明,当IMEF和IBEF取向一致时,亚胺键不仅可以为载流子迁移提供强大的驱动力,而且还能够有效地抑制载流子复合,进一步提高光生电子的利用率. 综上所述,本文提出了双电场叠加增强光生载流子高效分离的有效策略,为设计具有特定电场性质的COFs光催化材料提供了理论及实际参考.
Keyword ：
光催化 光催化 共价有机框架 共价有机框架 分子内电场 分子内电场 制氢 制氢 键内电场 键内电场
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| GB/T 7714 | 厉超 , 王朔 , 刘媛 et al. 共价有机框架双电场叠加实现高效光催化产氢 [J]. | 催化学报 , 2024 , 63 (8) : 164-175 . |
| MLA | 厉超 et al. "共价有机框架双电场叠加实现高效光催化产氢" . | 催化学报 63 . 8 (2024) : 164-175 . |
| APA | 厉超 , 王朔 , 刘媛 , 黄细河 , 庄严 , 吴舒鸿 et al. 共价有机框架双电场叠加实现高效光催化产氢 . | 催化学报 , 2024 , 63 (8) , 164-175 . |
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Metal nanoparticle (NP) cocatalysts are widely investigated for their ability to enhance the performance of photocatalytic materials; however, their practical application is often limited by the inherent instability under light irradiation. This challenge has catalyzed interest in exploring high-entropy alloys (HEAs), which, with their increased entropy and lower Gibbs free energy, provide superior stability. In this study, 3.5 nm-sized noble-metal-free NPs composed of a FeCoNiCuMn HEA are successfully synthesized. With theoretic calculation and experiments, the electronic structure of HEA in augmenting the catalytic CO2 reduction has been uncovered, including the individual roles of each element and the collective synergistic effects. Then, their photocatalytic CO2 reduction capabilities are investigated when immobilized on TiO2. HEA NPs significantly enhance the CO2 photoreduction, achieving a 23-fold increase over pristine TiO2, with CO and CH4 production rates of 235.2 and 19.9 mu mol g(-1) h(-1), respectively. Meanwhile, HEA NPs show excellent stability under simulated solar irradiation, as well high-energy X-ray irradiation. This research emphasizes the promising role of HEA NPs, composed of earth-abundant elements, in revolutionizing the field of photocatalysis.
Keyword ：
high-entropy alloy high-entropy alloy nanoparticle nanoparticle noble-metal-free noble-metal-free photocatalytic CO2 reduction photocatalytic CO2 reduction
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| GB/T 7714 | Huang, Haowei , Zhao, Jiwu , Guo, Hele et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction [J]. | ADVANCED MATERIALS , 2024 , 36 (26) . |
| MLA | Huang, Haowei et al. "Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction" . | ADVANCED MATERIALS 36 . 26 (2024) . |
| APA | Huang, Haowei , Zhao, Jiwu , Guo, Hele , Weng, Bo , Zhang, Hongwen , Saha, Rafikul Ali et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction . | ADVANCED MATERIALS , 2024 , 36 (26) . |
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To enhance the economy and society's sustainability, prioritizing innovative, green energy conversion methods is essential. The conversion of solar energy into chemical energy through photocatalysis represents a viable solution in the pursuit of sustainable energy resources despite low solar-to-energy conversion efficiency. In recent years, the immobilization of metal active centers in nanospace has been considered an important strategy to improve photocatalytic performance. Metal-organic frameworks (MOFs), covalent organic frameworks (COFs) and hydrogen-bonded organic frameworks (HOFs), as exciting reticular framework materials, have attracted much attention due to their advantages of large specific surface area, high porosity and tunable functionalization sites, which are considered promising carriers for immobilizing metal sites. This paper introduces the structural features and advantages of each framework in photocatalysis, highlighting their potential applications in water splitting (H2 or O2 evolution) and CO2 reduction. The review underscores the outstanding performance of metal-active sites within these frameworks. Finally, the current limitations and challenges of the reticular framework materials in photocatalysis are pointed out, and an outlook for future development is provided, which aims to inspire continued advancements in green energy solutions for a sustainable future. To enhance the economy and society's sustainability, prioritizing innovative, green energy conversion methods is essential.
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| GB/T 7714 | Wang, Shuo , Guo, Wei , Li, Chao et al. Immobilization of metal active centers in reticular framework materials for photocatalytic energy conversion [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (22) . |
| MLA | Wang, Shuo et al. "Immobilization of metal active centers in reticular framework materials for photocatalytic energy conversion" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 22 (2024) . |
| APA | Wang, Shuo , Guo, Wei , Li, Chao , Weng, Bo , Liu, Shuai , Han, Ning et al. Immobilization of metal active centers in reticular framework materials for photocatalytic energy conversion . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (22) . |
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Detoxicating materials of chemical warfare agents (CWAs) and their simulants play a critical role in reducing pollution contamination and environmental renovation. In this work, we present a simple strategy to prepare a core -shell structure Fe 3 O 4 /UiO-66-NH 2 /ILs@mSiO 2 using hydrogen bonding association and electrostatic forces. We performed disinfection studies on dimethyl 4-nitrophenyl phosphate (DMNP) and 2-chloroethyl ethyl sulfide (2-CEES). The synergistic effects of catalytic activations for CWAs, which reduce the electron transport distance and lower the reaction energy barrier, lead to an increase in hydrolysis and Fenton-like reactions efficiency. Eliminationing tests of DMNP and 2-CEES showed that the half-lives of the degradation reactions were 128.36 and 1.12 min, respectively, and the degradation efficiency did not decrease significantly after 4 cycles. This new type of structure could be magnetically separated within 60 s to facilitate material recovery and reuse. Moreover, the presence of a mesoporous silica shell made the catalyst particles to become biocompatible and environmentally friendly. The degradation pathways of the intermediates were revealed based on nuclear magnetic resonance spectroscopy (NMR), gaschromatography-mass spectrometry (GC -MS) and density functional theory (DFT) calculations. The effective combination of catalysts provided a facile strategy for developing multi-effect synergistic catalysts for the elimination of CWAs and other pollutants.
Keyword ：
Biocompatible Biocompatible Chemical Warfare Agents Chemical Warfare Agents Enrichment Capability Enrichment Capability Ionic Liquids Ionic Liquids Metal-Organic Frameworks Metal-Organic Frameworks
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| GB/T 7714 | Zhao, Hua , Li, Yu-Han , Zhao, Hongjie et al. In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
| MLA | Zhao, Hua et al. "In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations" . | SEPARATION AND PURIFICATION TECHNOLOGY 341 (2024) . |
| APA | Zhao, Hua , Li, Yu-Han , Zhao, Hongjie , Wang, Yi , Long, Jinlin , Sun, Ruize et al. In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
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Solar-driven methanation of carbon dioxide (CO2) with water (H2O) has emerged as an important strategy for achieving both carbon neutrality and fuel production. The selective methanation of CO2 was often hindered by the sluggish kinetics and the multiple competition of other C1 byproducts. To overcome this bottleneck, we utilized a biomass synthesis method to synthesize SiC rods and then constructed a direct Z-scheme heterojunction Co3O4/SiC catalyst. The substantial difference in work functions between SiC and Co3O4 served as a significant source of the charge driving force, facilitating the conversion of CO2 to CH4. The high-valent cobalt Co(IV) in Co3O4 acts as an active species to promote efficient dissociation of water. This favorable condition greatly enhanced the likelihood of a high concentration of electrons and protons around a single site on the catalyst surface for CO2 methanation. DFT calculation showed that the energy barrier of CO2 hydrogenation was significantly reduced at the Co3O4/SiC heterojunction interface, which changed the reaction pathway and completely converted the product from CO to CH4. The optimum CH4 evolution rate of Co3O4/SiC samples was 21.3 μmol g-1 h-1 with 100% selectivity. This study has an important guiding significance for the selective regulation of CO2 to CH4 products in photocatalysis applications. © 2024 American Chemical Society.
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| GB/T 7714 | Lin, M. , Cai, Q. , Xiao, Z. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity [J]. | Inorganic Chemistry , 2024 , 63 (31) : 14591-14601 . |
| MLA | Lin, M. et al. "Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity" . | Inorganic Chemistry 63 . 31 (2024) : 14591-14601 . |
| APA | Lin, M. , Cai, Q. , Xiao, Z. , Chen, H. , Wang, B. , Qiu, C. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity . | Inorganic Chemistry , 2024 , 63 (31) , 14591-14601 . |
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Battery-type faradaic materials are considered a class of promising electrodes for capacitive deionization (CDI) due to their superior ability to store ions through redox reactions. However, the desalination potential of such electrode materials has not been fully explored subject to the accessibility, conductivity, stability, etc. Herein, embedded battery material Ag nanoparticles is designed in capsule-structural units composed of graphene and constructed freestanding composite electrodes for CDI. Particularly, these Ag nanoparticles confined in interconnected graphene capsules can be both efficiently accessed by the electrolyte and rationally protected by the capsule networks, significantly unlocking their potential as desalination materials. Impressively, the optimized Ag-involved anodes can achieve an ultrahigh NaCl desalination capacity of approximate to 360 mg g-1 (approximate to 218 mg g-1 for Cl-) at 1.4 V and exhibit good cycling stability. Moreover, the as-designed anodes also have very competitive desalination capacities for other anions, such as SO2- 4 (approximate to 90 mg g-1) and CrO2- 4 (approximate to 77 mg g-1), suggesting the broad applicability of such Ag-involved electrodes. This work shows that the ingenious introduction of space-confined structures is an effective means of unlocking the desalination potential of Ag-based materials, opening up alternative avenues for the development of other high-performance battery-type desalination electrodes.
Keyword ：
binder-free binder-free capacitive deionization capacitive deionization capsule structure capsule structure confined redox confined redox faradaic electrodes faradaic electrodes
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| GB/T 7714 | Liu, Liyan , You, Shaojie , Liu, Haoyang et al. Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization [J]. | SMALL , 2024 , 21 (1) . |
| MLA | Liu, Liyan et al. "Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization" . | SMALL 21 . 1 (2024) . |
| APA | Liu, Liyan , You, Shaojie , Liu, Haoyang , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin et al. Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization . | SMALL , 2024 , 21 (1) . |
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