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学者姓名:孙再成

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Mechanistic Investigation into Single-Electron Oxidative Addition of Single-Atom Cu(I)-N4 Site: Revealing the Cu(I)-Cu(II)-Cu(I) Catalytic Cycle in Photochemical Hydrophosphinylation SCIE
期刊论文 | 2024 , 146 (12) , 8668-8676 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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Abstract :

Understanding the valency and structural variations of metal centers during reactions is important for mechanistic studies of single-atom catalysis, which could be beneficial for optimizing reactions and designing new protocols. Herein, we precisely developed a single-atom Cu(I)-N4 site catalyst via a photoinduced ligand exchange (PILE) strategy. The low-valent and electron-rich copper species could catalyze hydrophosphinylation via a novel single-electron oxidative addition (OA) pathway under light irradiation, which could considerably decrease the energy barrier compared with the well-known hydrogen atom transfer (HAT) and single electron transfer (SET) processes. The Cu(I)-Cu(II)-Cu(I) catalytic cycle, via single-electron oxidative addition and photoreduction, has been proven by multiple in situ or operando techniques. This catalytic system demonstrates high efficiency and requires room temperature conditions and no additives, which improves the turnover frequency (TOF) to 1507 h-1. In particular, this unique mechanism has broken through the substrate limitation and shows a broad scope for different electronic effects of alkenes and alkynes.

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GB/T 7714 Wang, Guanglin , Liu, Yichang , Zhang, Xiangyu et al. Mechanistic Investigation into Single-Electron Oxidative Addition of Single-Atom Cu(I)-N4 Site: Revealing the Cu(I)-Cu(II)-Cu(I) Catalytic Cycle in Photochemical Hydrophosphinylation [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (12) : 8668-8676 .
MLA Wang, Guanglin et al. "Mechanistic Investigation into Single-Electron Oxidative Addition of Single-Atom Cu(I)-N4 Site: Revealing the Cu(I)-Cu(II)-Cu(I) Catalytic Cycle in Photochemical Hydrophosphinylation" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 12 (2024) : 8668-8676 .
APA Wang, Guanglin , Liu, Yichang , Zhang, Xiangyu , Zong, Xupeng , Zhang, Xu , Zheng, Kun et al. Mechanistic Investigation into Single-Electron Oxidative Addition of Single-Atom Cu(I)-N4 Site: Revealing the Cu(I)-Cu(II)-Cu(I) Catalytic Cycle in Photochemical Hydrophosphinylation . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (12) , 8668-8676 .
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Highly Selective Photocatalytic Synthesis of Acetic Acid at 0-25 °C SCIE
期刊论文 | 2024 , 63 (42) | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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Acetic acid (AA), a vital compound in chemical production and materials manufacturing, is conventionally synthesized by starting with coal or methane through multiple steps including high-temperature transformations. Here we present a new synthesis of AA from ethane through photocatalytic selective oxidation of ethane by H2O2 at 0-25 degrees C. The catalyst designed for this process comprises g-C3N4 with anchored Pd1 single-atom sites. In situ studies and computational simulation suggest the immobilized Pd1 atom becomes positively charged under photocatalytic condition. Under photoirradiation, the holes on the Pd1 single-atom of OH-Pd1 circle plus ${{}<^>{\oplus }}$ /g-C3N4 serves as a catalytic site for activating a C-H instead of C-C of C2H6 with a low activation barrier of 0.14 eV, through a concerted mechanism. Remarkably, the selectivity for synthesizing AA reaches 98.7 %, achieved under atmospheric pressure of ethane at 0 degrees C. By integrating photocatalysis with thermal catalysis, we introduce a highly selective, environmentally friendly, energy-efficient synthetic route for AA, starting from ethane, presenting a promising alternative for AA synthesis. This integration of photocatalysis in low-temperature oxidation demonstrates a new route of selective oxidation of light alkanes. Acetic acid, a key intermediate compound, is synthesized by oxidization of ethane with H2O2 at 0 degrees C at ambient pressure through an integrated thermal catalysis and photocatalysis. The selectivity for producing acetic acid reaches 98.7 %. The positively charged Pd1 atom with an adsorbed OH group is the site for activating the first C-H of C2H6 with an energy barrier of only 0.14 eV. image

Keyword :

photocatalysis photocatalysis Ethane Ethane in situ/operando studies in situ/operando studies Single-atom catalysis Single-atom catalysis Acetic acid Acetic acid

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GB/T 7714 Zong, Xupeng , Chu, Yi-Chun , Tang, Yu et al. Highly Selective Photocatalytic Synthesis of Acetic Acid at 0-25 °C [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (42) .
MLA Zong, Xupeng et al. "Highly Selective Photocatalytic Synthesis of Acetic Acid at 0-25 °C" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 42 (2024) .
APA Zong, Xupeng , Chu, Yi-Chun , Tang, Yu , Li, Yuting , Wu, Xin-Ping , Sun, Zaicheng et al. Highly Selective Photocatalytic Synthesis of Acetic Acid at 0-25 °C . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (42) .
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Anammox Coupled with Photocatalyst for Enhanced Nitrogen Removal and the Activated Aerobic Respiration of Anammox Bacteria Based on cbb3-Type Cytochrome c Oxidase SCIE
期刊论文 | 2023 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
WoS CC Cited Count: 8
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This study is about anammox bacteria's physiologicalaptitudes, providing insights into applying solar energy for enhancedwastewater treatment. This study introduced photogenerated electrons into theanammoxsystem by coupling them to a g-C3N4 nanoparticlephotocatalyst. A high nitrogen removal efficiency (94.25%) was achieved,exceeding the biochemical limit of 89% imposed by anammox stoichiometry.Photogenerated electrons boosted anammox metabolic activity by empoweringkey enzymes (NIR, HZS, and WLP-related proteins) and triggered rapidalgal enrichment by enhancing the algal Calvin cycle, thus developingmultiple anammox-algae synergistic nitrogen removal processes.Remarkably, the homologous expression of cbb3-type cytochrome c oxidase(CcO) in anammox bacteria was discovered and reported in this studyfor the first time. This conferred aerobic respiration capabilityto anammox bacteria and rendered them the principal oxygen consumerunder 7.9-19.8 mg/L dissolved oxygen, originating from algalphotosynthesis. Additionally, photogenerated electrons selectivelytargeted the cb1 complex and cbb3-type CcO as activation sites whilemobilizing the RegA/B regulatory system to activate the expressionof cbb3-type CcO. Furthermore, cbb3-type CcO blocked oxidative stressin anammox by depleting intracellular oxygen, a substrate for reactiveoxygen species synthesis. This optimized the environmental sensitivityof anammox bacteria and maintained their high metabolic activity.This study expands our understanding of the physiological aptitudesof anammox bacteria and provides valuable insights into applying solarenergy for enhanced wastewater treatment.

Keyword :

anammox anammox enhancednitrogen removal enhancednitrogen removal photogenerated electrons photogenerated electrons solar energy solar energy meta-omics analysis meta-omics analysis

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GB/T 7714 Zhang, Li , Dong, Tingjun , Yang, Jiachun et al. Anammox Coupled with Photocatalyst for Enhanced Nitrogen Removal and the Activated Aerobic Respiration of Anammox Bacteria Based on cbb3-Type Cytochrome c Oxidase [J]. | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2023 .
MLA Zhang, Li et al. "Anammox Coupled with Photocatalyst for Enhanced Nitrogen Removal and the Activated Aerobic Respiration of Anammox Bacteria Based on cbb3-Type Cytochrome c Oxidase" . | ENVIRONMENTAL SCIENCE & TECHNOLOGY (2023) .
APA Zhang, Li , Dong, Tingjun , Yang, Jiachun , Hao, Shiwei , Sun, Zaicheng , Peng, Yongzhen . Anammox Coupled with Photocatalyst for Enhanced Nitrogen Removal and the Activated Aerobic Respiration of Anammox Bacteria Based on cbb3-Type Cytochrome c Oxidase . | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2023 .
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Recent advances in the heterogeneous photochemical synthesis of C-N bonds SCIE
期刊论文 | 2023 , 25 (13) , 5010-5023 | GREEN CHEMISTRY
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Over the few decades, photochemistry has received great attention and become a powerful tool in organic synthesis. Heterogeneous photocatalysts present complementary advantages in production, separation, catalyst recycling, and stability compared to the traditional homogeneous photocatalysts. In this review, we choose C-N bond formation as a typical coupling reaction and summarize the development of a heterogeneous catalytic system and its advantages. Titanium dioxide, semiconductor quantum dots, covalent organic frameworks, and carbon nitrides are discussed in detail as important heterogeneous photocatalysts. The combination and electron transfer pathway between heterogeneous catalysts and transition-metal catalysts are the focus of this review. These advances are not only limited to the C-N coupling, but also extend to other coupling reactions.

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GB/T 7714 Wang, Jinming , Liu, Yichang , Zong, Xupeng et al. Recent advances in the heterogeneous photochemical synthesis of C-N bonds [J]. | GREEN CHEMISTRY , 2023 , 25 (13) : 5010-5023 .
MLA Wang, Jinming et al. "Recent advances in the heterogeneous photochemical synthesis of C-N bonds" . | GREEN CHEMISTRY 25 . 13 (2023) : 5010-5023 .
APA Wang, Jinming , Liu, Yichang , Zong, Xupeng , Lei, Aiwen , Sun, Zaicheng . Recent advances in the heterogeneous photochemical synthesis of C-N bonds . | GREEN CHEMISTRY , 2023 , 25 (13) , 5010-5023 .
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The Formation Process and Mechanism of Carbon Dots Prepared from Aromatic Compounds as Precursors: A Review SCIE
期刊论文 | 2023 , 19 (31) | SMALL
WoS CC Cited Count: 53
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Fluorescent carbon dots are a novel type of nanomaterial. Due to their excellent optical properties, they have extensive application prospects in many fields. Studying the formation process and fluorescence mechanism of CDs will assist scientists in understanding the synthesis of CDs and guide more profound applications. Due to their conjugated structures, aromatic compounds have been continuously used to synthesize CDs, with emissions ranging from blue to NIR. There is a lack of a systematic summary of the formation process and fluorescence mechanism of aromatic precursors to form CDs. In this review, the formation process of CDs is first categorized into three main classes according to the precursor types of aromatic compounds: amines, phenols, and polycyclics. And then, the fluorescence mechanism of CDs synthesized from aromatic compounds is summarized. The challenges and prospects are proposed in the last section.

Keyword :

fluorescence mechanism fluorescence mechanism aromatic compounds aromatic compounds formation process formation process carbon dots carbon dots

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GB/T 7714 Xue, Shanshan , Li, Pengfei , Sun, Lu et al. The Formation Process and Mechanism of Carbon Dots Prepared from Aromatic Compounds as Precursors: A Review [J]. | SMALL , 2023 , 19 (31) .
MLA Xue, Shanshan et al. "The Formation Process and Mechanism of Carbon Dots Prepared from Aromatic Compounds as Precursors: A Review" . | SMALL 19 . 31 (2023) .
APA Xue, Shanshan , Li, Pengfei , Sun, Lu , An, Li , Qu, Dan , Wang, Xiayan et al. The Formation Process and Mechanism of Carbon Dots Prepared from Aromatic Compounds as Precursors: A Review . | SMALL , 2023 , 19 (31) .
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Highly efficient charge transfer from small-sized cadmium sulfide nanosheets to large-scale nitrogen-doped carbon for visible-light dominated hydrogen evolution SCIE
期刊论文 | 2023 , 630 , 260-268 | JOURNAL OF COLLOID AND INTERFACE SCIENCE
WoS CC Cited Count: 20
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Abstract :

Slow charge transfer and carrier recombination are key issues in photocatalytic reactions. The current solution is to load small-sized cocatalysts onto large-sized photocatalysts. Here a new strategy is pro-posed. Small-sized photocatalysts of cadmium sulfide (CdS) nanosheets are grown onto large-sized cocat-alysts of N-doped amorphous carbon (a-CN) to construct CdS @ a-CN photocatalysts. Photoluminescence spectra and transient photocurrent demonstrate that optimized CdS @ a-CN shows effective charge sep-aration compared with CdS. The corresponding photocatalytic H2 yield of optimized CdS @ a-CN is-244 lmol, which is 3.6 times higher than that of CdS. Besides, the hydrogen yield for CdS under visible-light irradiation is significantly improved from-44 lmol to-217 lmol for the optimized CdS @ a-CN. Our design strategy provides an effective way to construct photocatalytic systems with outstand-ing photocatalytic performance.(c) 2022 Published by Elsevier Inc.

Keyword :

N-doped carbon N-doped carbon Photocatalytic hydrogen Photocatalytic hydrogen CdS CdS Improved visible-light adsorption Improved visible-light adsorption

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GB/T 7714 Zhong, Jiaxing , Li, Yuanli , Zhang, Hang et al. Highly efficient charge transfer from small-sized cadmium sulfide nanosheets to large-scale nitrogen-doped carbon for visible-light dominated hydrogen evolution [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 630 : 260-268 .
MLA Zhong, Jiaxing et al. "Highly efficient charge transfer from small-sized cadmium sulfide nanosheets to large-scale nitrogen-doped carbon for visible-light dominated hydrogen evolution" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 630 (2023) : 260-268 .
APA Zhong, Jiaxing , Li, Yuanli , Zhang, Hang , Zhang, Zhenghan , Qi, Kezhen , Zhang, Hui et al. Highly efficient charge transfer from small-sized cadmium sulfide nanosheets to large-scale nitrogen-doped carbon for visible-light dominated hydrogen evolution . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 630 , 260-268 .
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Unravelling the adsorption and electroreduction performance of CO2 and N-2 over defective and B, P, Si-doped C(3)Ns: a DFT study SCIE
期刊论文 | 2023 , 25 (25) , 16952-16961 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
WoS CC Cited Count: 2
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Two-dimensional carbon-based materials have great potential for electrocatalysis. Herein, we screen 12 defective and doped C3N nanosheets by evaluating their CO2RR and NRR activity and selectivity vs. the HER based on density functional theory calculations. The calculation results suggest that all 12 C(3)Ns can enhance CO2 adsorption and activation. And P-N-V-C-C3N is the best electrocatalyst for the CO2RR towards HCOOH with U-L = -0.17 V, which is much more positive than most of the reported values. B-N-C3N and P-N-C3N are also good electrocatalysts that promote the CO2RR towards HCOOH (U-L = -0.38 V and -0.46 V). Moreover, we find that Si-C-C3N can reduce CO2 to CH3OH, adding an alternative option to the limited catalysts available for the CO2RR to CH3OH. Furthermore, B-C-V-C-C3N, B-C-V-N-C3N, and Si-C-V-N-C3N are promising electrocatalysts for the HER with |Delta G(H*)| <= 0.30 eV. However, only three C(3)Ns of B-C-V-C-C3N, Si-C-V-N-C3N, and Si-C-V-C-C3N can slightly improve N-2 adsorption. And none of the 12 C(3)Ns are found to be suitable for the electrocatalytic NRR because all the Delta e(NNH*) values are larger than the corresponding Delta G(H*) values. The high performance of C(3)Ns in the CO2RR stems from the altered structure and electronic properties, which result from the introduction of vacancies and doping elements into C3N. This work identifies suitable defective and doped C(3)Ns for excellent performance in the electrocatalytic CO2RR, which will inspire relevant experimental studies to further explore C(3)Ns for electrocatalysis.

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GB/T 7714 Wang, Dandan , Liu, Xueting , Yang, Huiru et al. Unravelling the adsorption and electroreduction performance of CO2 and N-2 over defective and B, P, Si-doped C(3)Ns: a DFT study [J]. | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (25) : 16952-16961 .
MLA Wang, Dandan et al. "Unravelling the adsorption and electroreduction performance of CO2 and N-2 over defective and B, P, Si-doped C(3)Ns: a DFT study" . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS 25 . 25 (2023) : 16952-16961 .
APA Wang, Dandan , Liu, Xueting , Yang, Huiru , Zhao, Ziang , Liu, Yucheng , Qu, Xin et al. Unravelling the adsorption and electroreduction performance of CO2 and N-2 over defective and B, P, Si-doped C(3)Ns: a DFT study . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (25) , 16952-16961 .
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Fe2Mo3O8/XC-72 electrocatalyst for enhanced electrocatalytic nitrogen reduction reaction under ambient conditions SCIE
期刊论文 | 2022 , 15 (7) , 5940-5945 | NANO RESEARCH
WoS CC Cited Count: 18
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To perform the electrochemical nitrogen reduction reaction (NRR) under milder conditions for sustainable ammonia production, electrocatalysts should exhibit high selectivity, activity, and durability. However, the key restrictions are the highly stable N N triple bond and the competitive hydrogen evolution reaction (HER), which make it difficult to adsorb and activate N-2 on the surface of electrocatalysts, leading to a low ammonia yield and Faraday efficiency. Inspired by the enzymatic nitrogenase process and using the Fe-Mo as the active center, here we report supported Fe2Mo3O8/XC-72 as an effective and durable electrocatalyst for the NRR. Fe2Mo3O8/XC-72 exhibited NRR activity with an NH3 yield of 30.4 mu g.h(-1).mg(-1) (-0.3 V) and a Faraday efficiency of 8.2% (-0.3 V). Theoretical calculations demonstrated that the electrocatalytic nitrogen fixation mechanism involved the Fe atom in the Fe2Mo3O8/XC-72 electrocatalyst acting as the main active site in the enzymatic pathway (*NH2 ->*NH3), which activated nitrogen molecules and promoted the NRR performance.

Keyword :

Fe2Mo3O8/XC-72 electrocatalyst Fe2Mo3O8/XC-72 electrocatalyst nitrogen reduction reaction (NRR) nitrogen reduction reaction (NRR) density functional theory calculations density functional theory calculations

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GB/T 7714 Liu, Guohua , Niu, Lijuan , Ma, Zhixue et al. Fe2Mo3O8/XC-72 electrocatalyst for enhanced electrocatalytic nitrogen reduction reaction under ambient conditions [J]. | NANO RESEARCH , 2022 , 15 (7) : 5940-5945 .
MLA Liu, Guohua et al. "Fe2Mo3O8/XC-72 electrocatalyst for enhanced electrocatalytic nitrogen reduction reaction under ambient conditions" . | NANO RESEARCH 15 . 7 (2022) : 5940-5945 .
APA Liu, Guohua , Niu, Lijuan , Ma, Zhixue , An, Li , Qu, Dan , Wang, Dandan et al. Fe2Mo3O8/XC-72 electrocatalyst for enhanced electrocatalytic nitrogen reduction reaction under ambient conditions . | NANO RESEARCH , 2022 , 15 (7) , 5940-5945 .
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PD/A原位耦合藻类实现深度脱氮除磷的方法及装置 incoPat
专利 | 2022-04-13 | CN202210385684.6
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本发明提了一种PD/A原位耦合藻类实现深度脱氮除磷的方法和装置,所述方法包括将污水送入短程反硝化‑厌氧氨氧化反应区进行处理的步骤;在短程反硝化‑厌氧氨氧化反应区富集有藻类并投加有光催化材料;向污水中投加乙酸作为碳源;处理过程中使用可见光对反应区进行光照,通过调节光照参数控制藻类数量,使反应区的溶解氧浓度保持为0.9‑1.5mg/L,原位生成氨氧化菌。本发明通过向PD/A反应区中投加光催化材料,促进藻类于生物反应器内原位富集,同时调节光照条件的手段,创造并维持微氧环境,促进AOB菌群原位生长,形成菌藻共生的PD/A‑PN/A体系,强化体系脱氮除磷,实现氮磷的同步高效去除。

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GB/T 7714 张莉 , 董亭君 , 孙再成 et al. PD/A原位耦合藻类实现深度脱氮除磷的方法及装置 : CN202210385684.6[P]. | 2022-04-13 .
MLA 张莉 et al. "PD/A原位耦合藻类实现深度脱氮除磷的方法及装置" : CN202210385684.6. | 2022-04-13 .
APA 张莉 , 董亭君 , 孙再成 , 杨嘉春 , 豆全浩 . PD/A原位耦合藻类实现深度脱氮除磷的方法及装置 : CN202210385684.6. | 2022-04-13 .
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Recent advances of carbon dots as new antimicrobial agents
期刊论文 | 2022 , 3 (2) , 226-248 | SMARTMAT
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Due to the COVID-19 pandemic, many rapid antimicrobial agents have developed intensively. Carbon dots (CDs), a new type of carbon-based nanomaterials, shows great potential against emerging infectious diseases and antimicrobial-resistant infections due to their unique optical properties, excellent biocompatibility, and easy surface modification. With the definition of the CDs structure and properties, synthesis, and characteristic technology improvement, the research on the CDs as antimicrobial agents has made significant progress. However, the lack of high repeatable and exact preparation methods, and the regular antimicrobial activity make it far from practical application. In this review, we summarize the most recent progress and challenges of CDs antimicrobial. First, an overview of the characteristics and properties is given, and the advantage of CDs applied to antimicrobial is further discussed. Then, it focuses on research progress on antimicrobial mechanisms under different conditions, the critical factors affecting their antimicrobial activity, and the practical antimicrobial applications. Finally, the main challenges and future research perspectives of antimicrobial CDs are proposed.

Keyword :

antimicrobial activity antimicrobial activity photodynamic effect photodynamic effect reactive oxygen species reactive oxygen species antimicrobial antimicrobial carbon dots carbon dots

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GB/T 7714 Li, Pengfei , Sun, Lu , Xue, Shanshan et al. Recent advances of carbon dots as new antimicrobial agents [J]. | SMARTMAT , 2022 , 3 (2) : 226-248 .
MLA Li, Pengfei et al. "Recent advances of carbon dots as new antimicrobial agents" . | SMARTMAT 3 . 2 (2022) : 226-248 .
APA Li, Pengfei , Sun, Lu , Xue, Shanshan , Qu, Dan , An, Li , Wang, Xiayan et al. Recent advances of carbon dots as new antimicrobial agents . | SMARTMAT , 2022 , 3 (2) , 226-248 .
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