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学者姓名：汪颖
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Abstract ：
This work proposes a sigma-pi hyperconjugation strategy to establish interlayer charge transport channels (CTC) in supramolecular organic nanostructures. A series of ullazine-based molecular semiconductors were designed and synthesized successfully by engineering end groups to demonstrate the sigma-pi hyperconjugation that unlocks the quantum confinement of photogenerated charges in pi-conjugated planes. Ullazine grafted with tert-butyl (U-t-Bu) showed a J-cross-stacking model in which the cross-stacked U-t-Bu molecular pair smoothly glides along the elongated dimension, forming a Z-schemed interlayer CTC by sigma-pi hyperconjugations between C-H sigma-bonds of tert-butyl end group and pi-bonds of ullazines in adjacent layers along the stacking dimension. Consequently, upon photoexcitation of ullazine-based supramolecular nanoaggregates in aqueous solution, the formed Frenkel excitons are dissociated to charge-separated excitons by the interlayer charge separation channels, undergoing an ultrafast charge transfer within 0.58 ps and an ultrafast charge separation within 0.67 ps. The Z-schemed charge separation between adjacent layers leads to a significantly enhanced hydrogen yield over U-t-Bu/PVP/Pt, with a hydrogen evolution rate of 369.9 mu molg-1h-1 and an apparent quantum yield of 1.46% at 420 nm. It is 3.8-fold larger than that of ullazine modified with methoxy (U-OMe), without the sigma-pi hyperconjugation.
Keyword ：
exciton dynamics exciton dynamics HER HER hyperconjugation effect hyperconjugation effect photocatalysis photocatalysis supramolecule supramolecule
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| GB/T 7714 | Yang, Qin , Li, Wanqing , Wang, Ying et al. σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution [J]. | ACS CATALYSIS , 2025 , 15 (4) : 3267-3275 . |
| MLA | Yang, Qin et al. "σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution" . | ACS CATALYSIS 15 . 4 (2025) : 3267-3275 . |
| APA | Yang, Qin , Li, Wanqing , Wang, Ying , Zhuang, Yan , Wu, Shuhong , Wang, Shuo et al. σ-π Hyperconjugation Unlocks Interlayer Charge Separation of Ullazine-Based Supramolecular Nanostructures for Photocatalytic Hydrogen Evolution . | ACS CATALYSIS , 2025 , 15 (4) , 3267-3275 . |
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Abstract ：
H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost-effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three-component photocatalyst, Co(5 %)-HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O2 and H2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.
Keyword ：
carbon nitride chips carbon nitride chips overall water splitting overall water splitting photocatalytic photocatalytic PPOWS decoupling PPOWS decoupling reaction mechanism reaction mechanism
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| GB/T 7714 | Liu, Dan , Xu, Huihui , Shen, Jinni et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
| MLA | Liu, Dan et al. "Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) . |
| APA | Liu, Dan , Xu, Huihui , Shen, Jinni , Wang, Xun , Qiu, Chengwei , Lin, Huaxiang et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
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The persistent threats posed by toxic chemical warfare agents (CWAs) such as mustard gas (bis(2-chloroethyl) sulfide, HD) and bacterial contaminants demand the development of innovative, sustainable mitigation strategies. Photocatalytic processes that generate reactive oxygen species (ROS) offer a promising dual-functional approach for both chemical detoxification and antibacterial defense. In this study, two structurally analogous covalent organic frameworks (COFs), BPY-COF and BD-COF, are synthesized using benzotrithiophene as the donor unit paired with bipyridine and biphenyl, respectively. These COFs exhibit high crystallinity, broad-spectrum light absorption, and efficient charge carrier transport, with BPY-COF demonstrating superior performance due to the incorporation of heteroatoms. BPY-COF achieved ultrafast detoxification of the mustard gas simulant 2-chloroethyl ethyl sulfide (CEES) with a half-life of 35 min and 100% selectivity for 2-chloroethyl sulfoxide (CEESO) under white LED light, outperforming BD-COF. Additionally, electrospun composite fibers containing 40 wt.% BPY-COF maintained comparable CEES degradation rates and exhibited over 99% antibacterial efficiency against Escherichia coli and Bacillus subtilis within 60 min. These findings highlight the potential of BPY-COF as a multifunctional photocatalyst for integrated applications in chemical detoxification and antibacterial defense, addressing critical challenges in public health and safety.
Keyword ：
antibacterial antibacterial charge transfer charge transfer covalent organic frameworks covalent organic frameworks photocatalytic degradation photocatalytic degradation
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| GB/T 7714 | Zhu, Yongchao , Qin, Liyang , Yang, Mingyuan et al. Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense [J]. | SMALL , 2025 , 21 (12) . |
| MLA | Zhu, Yongchao et al. "Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense" . | SMALL 21 . 12 (2025) . |
| APA | Zhu, Yongchao , Qin, Liyang , Yang, Mingyuan , Shi, Zhicheng , Chen, Hongxuan , Wen, Na et al. Dual-Functional Benzotrithiophene-Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense . | SMALL , 2025 , 21 (12) . |
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Converting clean solar energy into chemical energy through artificial photosynthesis is an effective solution to solve the energy and environmental issues. Here, we report a Cs3Bi2Br9/Bi2WO6 (CBB/BWO) Z-scheme heterojunction constructed via electrostatic self-assembly, which facilitates efficient separation of photogenerated carriers and ensures the corresponding redox capacity of both components. By sharing Bi atoms, a Br-Bi-O bond is established between CBB and BWO, serving as an "electron bridge". The electrons generated by BWO are efficiently channeled to CBB through the heterojunction-formed "electron bridge", thereby achieving effective photocatalytic CO2 reduction. Under simulated sunlight conditions, it exhibits the highest CO yield of 72.52 mu mol g(-1) (without the addition of any precious metal, photosensitizers or sacrifices), which is approximately 7-fold and 18-fold greater than that of pure CBB and BWO, respectively. This work provides a more profound comprehension of the regulation of electron transfer through interfacial chemical bonds, thereby proposing a promising strategy for the development of efficient heterojunction photocatalysts for CO2 photoreduction.
Keyword ：
Bi2WO6 Bi2WO6 CO2 reduction CO2 reduction Perovskite Perovskite Photocatalysis Photocatalysis Z-scheme Z-scheme
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| GB/T 7714 | Liu, Haolan , Sun, Jingjing , Lin, Qianying et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction [J]. | CHEMCATCHEM , 2024 , 16 (22) . |
| MLA | Liu, Haolan et al. "An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction" . | CHEMCATCHEM 16 . 22 (2024) . |
| APA | Liu, Haolan , Sun, Jingjing , Lin, Qianying , Wang, Ying , Wang, Shuo , Wang, Shuowen et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction . | CHEMCATCHEM , 2024 , 16 (22) . |
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Bacterial infections are a major public health challenge around the world. The development of novel surface coatings that effectively inhibit bacterial adhesion, proliferation and growth is a critical step in addressing this global challenge. Photocatalytic antibacterial therapy has proven to be an effective approach and has received increasing attention. However, it is still a challenge to obtain coatings with both antibacterial adhesion and durable photocatalytic antibacterial functions. Herein, an acridine-based coating with antibacterial adhesion and photocatalytic antibacterial properties was prepared by simple methods (i.e., spin-coating, spray-coating, and drop-coating) and can be applied to various substrates. The bacterial anti-adhesion test results showed that the coating could effectively prevents the adhesion of Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), and Pseudomonas aeruginosa (P. aeruginosa), indicating the strong anti-fouling capability. The acridine-based coating demonstrated durable photocatalytic antimicrobial activity, remaining 99.3 % antibacterial effective against all three bacterial strains even after 30 days exposed to visible light. The coating can significantly reduce or eliminate the risk of contamination and cross-contamination, making it ideal for use in public healthcare environments.
Keyword ：
Antibacterial Antibacterial Anti-fouling Anti-fouling Coating Coating Photocatalytic Photocatalytic
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| GB/T 7714 | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial [J]. | PROGRESS IN ORGANIC COATINGS , 2024 , 194 . |
| MLA | Kang, Linfeng et al. "Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial" . | PROGRESS IN ORGANIC COATINGS 194 (2024) . |
| APA | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan , Hu, Ke , Lin, Yihui , Zhu, Yongchao et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial . | PROGRESS IN ORGANIC COATINGS , 2024 , 194 . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword ：
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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| GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
| MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
| APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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The electrocatalytic conversion of inert CO2 to value-added chemical fuels powered by renewable energy is one of the benchmark approaches to address excessive carbon emissions and achieve carbon-neutral energy restructuring. However, the adsorption/activation of supersymmetric CO2 is facing insurmountable challenges that constrain its industrial-scale applications. Here, this theory-guided study confronts these challenges by leveraging the synergies of bimetallic sites and defect engineering, where pyrochlore-type semiconductor A(2)B(2)O(7) is employed as research platform and the conversion of CO2-to-HCOOH as the model reaction. Specifically, defect engineering intensified greatly the chemisorption-induced CO2 polarization via the bimetallic coordination, thermodynamically beneficial to the HCOOH production via the *HCO2 intermediate. The optimal V-BSO-430 electrocatalyst with abundant surface oxygen vacancies achieved a superior HCOOH yield of 116.7 mmol h(-1) cm(-2) at -1.2 V-RHE, rivalling the incumbent similar reaction systems. Furthermore, the unique catalytic unit featured with a Bi-1-Sn-Bi-2 triangular structure, which is reconstructed by defect engineering, and altered the pathway of CO2 adsorption and activation to allow the preferential affinity of the suspended O atom in *HCO2 to H. As a result, V-BSO-430 gave an impressive FEHCOOH of 93% at -1.0 V-RHE. This study held promises for inspiring the exploration of bimetallic materials from the massive semiconductor database.
Keyword ：
A(2)B(2)O(7) A(2)B(2)O(7) bimetallic sites bimetallic sites CO2 reduction CO2 reduction electrocatalysis electrocatalysis pyrochlore pyrochlore
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| GB/T 7714 | Zhao, Jiwu , Wang, Jiashun , Xue, Lan et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Zhao, Jiwu et al. "Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH" . | SMALL 20 . 38 (2024) . |
| APA | Zhao, Jiwu , Wang, Jiashun , Xue, Lan , Wang, Ying , Wen, Na , Huang, Haowei et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH . | SMALL , 2024 , 20 (38) . |
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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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Main group Bi-based materials have gained popularity as N2 reduction reaction (NRR) photo/electrocatalysts due to their ability to inhibit competitive H2 evolution reactions (HER) and the unique N2 adsorption activities. The introduction of defects in Bi-based catalysts represents a highly effective strategy for enhancing light absorption, promoting efficient separation of photogenerated carriers, optimizing the activity of free radicals, regulating electronic structure, and improving catalytic performance. In this review, we outline the various applications of state of the defect engineering in Bi-based catalysts and elucidate the impact of vacancies on NRR performance. In particular, the types of defects, methods of defects tailoring, advanced characterization techniques, as well as the Bi-based catalysts with abundant defects and their corresponding catalytic behavior in NRR were elucidated in detail. Finally, the main challenges and opportunities for future development of defective Bi-based NRR catalysts are discussed, which provides a comprehensive theoretical guidance for this field. In this review, the categories, construction strategies and advanced characterization techniques of defect engineering in current Bi-based NRR catalysts are summarized, and the main challenges and opportunities for the future development of defective Bi-based NRR catalysts are discussed, providing a comprehensive theoretical guidance for this field. image
Keyword ：
Bismuth Bismuth Defects Defects Doping Doping Materials science Materials science Nitrogen fixation Nitrogen fixation Photocatalysis Photocatalysis
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| GB/T 7714 | Lv, Shuhua H. , Wang, Ying , Wang, Debao B. et al. Defect Engineering in Bi-based Photo/electrocatalysts for Nitrogen Reduction to Ammonia [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2024 , 30 (37) . |
| MLA | Lv, Shuhua H. et al. "Defect Engineering in Bi-based Photo/electrocatalysts for Nitrogen Reduction to Ammonia" . | CHEMISTRY-A EUROPEAN JOURNAL 30 . 37 (2024) . |
| APA | Lv, Shuhua H. , Wang, Ying , Wang, Debao B. , Song, Caixia X. . Defect Engineering in Bi-based Photo/electrocatalysts for Nitrogen Reduction to Ammonia . | CHEMISTRY-A EUROPEAN JOURNAL , 2024 , 30 (37) . |
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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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