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Efficient Photocatalytic CO2 Reduction in Ellagic Acid-Based Covalent Organic Frameworks

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 2024年第23期146卷 16229-16236页

作者： lin, Wan lin, fuwen lin, Jing Xiao, Zhiwei Yuan, Daqiang Wang, Yaobing Chinese Acad Sci CAS Key Lab Design & Assembly Funct Nanostruct Fuzhou 350002 Fujian Peoples R China Chinese Acad Sci Fujian Inst Res Struct Matter Fujian Prov Key Lab Nanomat State Key Lab Struct Chem Fuzhou 350002 Fujian Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China Fujian Normal Univ Coll Chem & Mat Sci Fuzhou 350007 Peoples R China Fujian Sci & Technol Innovat Lab Optoelect Informa Fuzhou 350108 Fujian Peoples R China

Employing covalent organic frameworks (COFs) for the photocatalytic CO2 reduction reaction (CDRR) to generate high-value chemical fuels and mitigate greenhouse gas emissions represents a sustainable catalytic conversion approach. However, achieving superior photocatalytic CDRR performance is hindered by the challenges of low charge separation efficiency, poor stability, and high preparation costs associated with COFs. Herein, in this work, we utilized perfluorinated metallophthalocyanine (MPcF16) and the organic biomolecule compound ellagic acid (EA) as building blocks to actualize functional covalent organic frameworks (COFs) named EPM-COF (M = Co, Ni, Cu). The designed EPCo-COF, featuring cobalt metal active sites, demonstrated an impressive CO production rate and selectivity in the photocatalytic CO2 reduction reaction (CDRR). Moreover, following alkaline treatment (EPCo-COF-AT), the COF exposed carboxylic acid anion (COO-) and hydroxyl group (OH), thereby enhancing the electron-donating capability of EA. This modification achieved a heightened CO production rate of 17.7 mmol g(-1) h(-1) with an outstanding CO selectivity of 97.8% in efficient photocatalytic CDRR. Theoretical calculations further illustrated that EPCo-COF-AT functionalized with COO- and OH can effectively alleviate the energy barriers involved in the CDRR process, which facilitates the proton-coupled electron transfer processes and enhances the photocatalytic performance on the cobalt active sites within EPCo-COF-AT.

关键词： Charge transfer Cobalt Covalent organic frameworks Metals Separation science

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Photo-Driven Ammonia Synthesis via a Proton-Mediated Photoelectrochemical Device

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 2025年第8期64卷 e202422869页

作者： lin, Wan Chen, Jiajie Zhang, Xiang lin, Jing lin, fuwen Huang, ShenXia Wang, Yaobing Chinese Acad Sci CAS Key Lab Design & Assembly Funct Nanostruct Fuzhou 350002 Fujian Peoples R China Chinese Acad Sci Fujian Prov Key Lab Nanomat State Key Lab Struct Chem Fujian Inst Res Struct Matter Fuzhou 350002 Fujian Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China Fuzhou Univ Coll Chem Fuzhou 350116 Fujian Peoples R China Fujian Normal Univ Coll Chem & Mat Sci Fuzhou 350007 Peoples R China Fujian Sci & Technol Innovat Lab Optoelect Inform Fuzhou 350108 Fujian Peoples R China Univ Chinese Acad Sci Fujian Coll Fuzhou 350002 Peoples R China

N-2 reduction reaction (NRR) by light is an energy-saving and sustainable ammonia (NH3) synthesis technology. However, it faces significant challenges, including high energy barriers of N-2 activation and unclear catalytic active sites. Herein, we propose a strategy of photo-driven ammonia synthesis via a proton-mediated photoelectrochemical device. We used redox-catalysis covalent organic framework (COF), with a redox site (-C=O) for H+ reversible storage and a catalytic site (porphyrin Au) for NRR. In the proton-mediated photoelectrochemical device, the COF can successfully store e(-) and H+ generated by hydrogen oxidation reaction, forming COF-H. Then, these stored e(-) and H+ can be used for photo-driven NRR (108.97 umol g(-1)) under low proton concentration promoted by the H-bond network formed between -OH in COF-H and N-2 on Au, which enabled N-2 hydrogenation and NH3 production, establishing basis for advancing artificial photosynthesis and enhancing ammonia synthesis technology.

关键词： Photo-driven ammonia synthesis Proton-mediated N-2 reduction reaction Covalent organic framework Photoelectrochemical device

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Morpholine-linked metal-phthalocyanine covalent organic frameworks for enhanced photocatalytic CO2 reduction

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JOURNAL OF MATERIALS CHEMISTRY A 2025年第5期13卷 3287-3294页

作者： lin, fuwen lin, Wan lin, Jing Xiao, Zhiwei Hui, Yangdan Chen, Junlan Wang, Yaobing Chinese Acad Sci CAS Key Lab Design & Assembly Funct Nanostruct Fujian Prov Key Lab Nanomat State Key Lab Struct ChemFujian Inst Res Struct M Fuzhou 350002 Fujian Peoples R China Fujian Normal Univ Coll Chem & Mat Sci Fuzhou 350007 Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China Fujian Sci & Technol Innovat Lab Optoelect Informa Fuzhou 350108 Fujian Peoples R China Univ Chinese Acad Sci Fujian Coll Fuzhou 350002 Peoples R China

Developing technology of artificial photosynthetic CO2 reduction is essential to improve the issues of global carbon emissions and climate change. However, it is still limited by the low charge separation efficiency and poor transport capacity of photocatalysts. Herein, two novel morpholine-linked metal-phthalocyanine COFs, Co-DA-COF and Co-DB-COF, were synthesized through the nucleophilic aromatic substitution reaction of cobalt perfluorophthalocyanine (CoPcF16) with 2,5-phenylenediamine-1,4-diphenol (DHA) and 3,3 '-dihydroxybenzidine (DHB). The introduction of morpholine bonds and the specific photosensitivity of metal phthalocyanines resulted in remarkable photocatalytic CO2 reduction reaction (CDRR) activity. Notably, Co-DB-COF exhibited enhanced electron delocalization owing to its expanded pi-conjugated system, which facilitated the process of separating and transporting photogenerated charge carriers. This resulted in a notable rate of CO production of 25.7 mmol g-1 h-1, exhibiting a selectivity of 92.3% and an AQE of 0.65% at 450 nm, which surpasses the majority of previously documented visible-light-driven COF-based photocatalysts. This work demonstrated the capability of morpholine-linked metal-phthalocyanine COFs in CO2 photocatalytic conversion, providing fresh insights for designing novel artificial photosynthesis catalysts.

关键词： Substitution reactions

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Redox-Mediated TEMPO-Based Donor-Acceptor Covalent Organic Framework for Efficient Photo-Induced Hydrogen Peroxide Generation

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 2025年第0期64卷 e202500924页

作者： Chen, Junlan Yan, Shichen Wang, Futong lin, fuwen lin, Jing Borse, Rahul Anil Wang, Yaobing Chinese Acad Sci Fujian Inst Res Struct Matter CAS Key Lab Design & Assembly Funct Nanostruct State Key Lab Struct Chem Fuzhou 350002 Fujian Peoples R China Chinese Acad Sci Fujian Inst Res Struct Matter Fujian Prov Key Lab Nanomat State Key Lab Struct Chem Fuzhou 350002 Fujian Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China Fujian Sci & Technol Innovat Lab Optoelect Informa Fuzhou 350108 Fujian Peoples R China

Molecular engineering of covalent organic frameworks (COFs) offers an alternative approach to conventional anthraquinone oxidation via photo-induced H2O2 production from O2 reduction. Despite their potential, reported photocatalysts suffer limited proton mobility, low selectivity, and insufficient charge separation and utilization. Herein, we report a nitroxyl radical (TEMPO) decorated two-dimensional (2D) donor-acceptor (D-A)-COF photocatalyst via a one-pot strategy. Under visible light irradiation, highly crystalline TAPP-TPDA-TEMPO-COF (TT-T-COF) exhibits a remarkable photocatalytic H2O2 yield of 10066 mu mol g-1 h-1 in two-phase water-benzyl alcohol (10 % BA) system through direct two-electron (2e-) pathway. The mechanistic study by DFT calculations and in situ DRIFT spectra suggests Yeager-type adsorption of *O2 & sdot;- intermediate on the nitroxyl radical site (N-O & sdot;). The efficient photocatalytic performance and stability of TT-T-COF are attributed to the involvement of the nitroxyl radical, which enhances selective O2 adsorption, establishes a distinct electron density distribution, and facilitates photogenerated charge separation compared to TT-HT-COF and TT-COF counterparts. This study uncovers a new perspective for constructing metal-free, redox-mediated radical-based COFs for sustainable energy conversion, storage, and biomedical applications.

关键词： radical covalent organic frameworks oxygen reduction reaction TEMPO-based photocatalyst density functional theory

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Photo-Driven Ammonia Synthesis via a Proton-Mediated Photoelectrochemical Device

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Angewandte Chemie 2025年第8期137卷

作者： Wan lin Jiajie Chen Xiang Zhang Jing lin fuwen lin ShenXia Huang Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian College University of Chinese Academy of Sciences Fuzhou 350002 P. R. China College of Chemistry Fuzhou University Fuzhou 350116 Fujian P. R. China. Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 China

N 2 reduction reaction (NRR) by light is an energy-saving and sustainable ammonia (NH 3 ) synthesis technology. However, it faces significant challenges, including high energy barriers of N 2 activation and unclear catalytic active sites. Herein, we propose a strategy of photo-driven ammonia synthesis via a proton-mediated photoelectrochemical device. We used redox-catalysis covalent organic framework (COF), with a redox site (−C=O) for H + reversible storage and a catalytic site (porphyrin Au) for NRR. In the proton-mediated photoelectrochemical device, the COF can successfully store e − and H + generated by hydrogen oxidation reaction, forming COF−H. Then, these stored e − and H + can be used for photo-driven NRR (108.97 umol g −1 ) under low proton concentration promoted by the H-bond network formed between −OH in COF−H and N 2 on Au, which enabled N 2 hydrogenation and NH 3 production, establishing basis for advancing artificial photosynthesis and enhancing ammonia synthesis technology.

关键词： Photo-driven ammonia synthesis Proton-mediated N2 reduction reaction Covalent organic framework Photoelectrochemical device

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Trap suppression in ordered organic photovoltaic heterojunctions

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CHEMICAL COMMUNICATIONS 2024年第4期60卷 364-373页

作者： He, Dan Li, Yawen Zhao, fuwen lin, Yuze Cent South Univ Coll Chem & Chem Engn Changsha 410083 Peoples R China Chinese Acad Sci Inst Chem Beijing Natl Lab Mol Sci CAS Key Lab Organ Solids Beijing 100190 Peoples R China Univ Chinese Acad Sci Beijing 100190 Peoples R China

The high trap density (generally 1016-1018 cm-3) in organic solar cells (OSCs) brings about the localization of charge carriers and reduced charge carrier lifetime, mainly due to the weak intermolecular interactions of organic semiconductors resulting in their relatively poor crystallinity, which leads to low charge carrier mobilities and intense non-radiative recombination, thus impeding the further improvement of power conversion efficiencies (PCEs). Therefore, trap suppression is crucial to boost the performance of OSCs, and improving the crystallinity of donor/acceptor materials and enhancing the molecular order in devices can contribute to the trap suppression in OSCs. In this feature article, we summarize the recent advances of trap suppression in OSCs by material design and device engineering, and further outline possible development directions for trap suppression to enhance PCEs of OSCs. High trap density in organic solar cells leads to the localized charge carrier and reduced carrier lifetime, limiting device efficiency. Here we summarize the recent advances of trap suppression by material design and device engineering.

关键词： Organic solar cells

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Redox-Mediated TEMPO-Based Donor-Acceptor Covalent Organic Framework for Efficient Photo-Induced Hydrogen Peroxide Generation

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Angewandte Chemie 2025年

作者： Junlan Chen Dr. Shichen Yan Futong Wang fuwen lin Dr. Jing lin Dr. Rahul Anil Borse Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

Molecular engineering of covalent organic frameworks (COFs) offers an alternative approach to conventional anthraquinone oxidation via photo-induced H 2 O 2 production from O 2 reduction. Despite their potential, reported photocatalysts suffer limited proton mobility, low selectivity, and insufficient charge separation and utilization. Herein, we report a nitroxyl radical (TEMPO) decorated two-dimensional (2D) donor-acceptor (D-A)-COF photocatalyst via a one-pot strategy. Under visible light irradiation, highly crystalline TAPP-TPDA-TEMPO-COF ( TT-T-COF ) exhibits a remarkable photocatalytic H 2 O 2 yield of 10066 μmol g −1 h −1 in two-phase water-benzyl alcohol (10 % BA) system through direct two-electron (2 e − ) pathway. The mechanistic study by DFT calculations and in situ DRIFT spectra suggests Yeager-type adsorption of *O 2 ⋅ − intermediate on the nitroxyl radical site (N−O⋅). The efficient photocatalytic performance and stability of TT-T-COF are attributed to the involvement of the nitroxyl radical, which enhances selective O 2 adsorption, establishes a distinct electron density distribution, and facilitates photogenerated charge separation compared to TT-HT-COF and TT-COF counterparts. This study uncovers a new perspective for constructing metal-free, redox-mediated radical-based COFs for sustainable energy conversion, storage, and biomedical applications.

关键词： radical covalent organic frameworks oxygen reduction reaction TEMPO-based photocatalyst density functional theory

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Preparation of iodine-131 labeled Polyvinyl alcohol-collagen microspheres for radioembolization therapy of liver tumors

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SCIENTIFIC REPORTS 2025年第1期15卷 1-10页

作者： Li, Yuhao Cai, Huawei Xing, Yikai Pang, fuwen Li, lin Sichuan Univ West China Hosp Dept Nucl Med Chengdu Sichuan Peoples R China Sichuan Univ West China Hosp West China Sch Med Chengdu Sichuan Peoples R China Shenzhen Tradit Chinese Med Hosp Dept Intervent Shenzhen Guangdong Peoples R China

Transarterial radioembolization using radionuclide-labeled microspheres has shown efficacy in the treatment of hepatocellular carcinoma (HCC). In this study, a novel formulation of Polyvinyl alcohol-collagen microspheres (PCMs) with an optimal settling rate is developed. Fourier-transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM) analyses confirm that the PCMs have uniform morphology with diameters ranging from 20 to 30 mu m. These microspheres are successfully labeled with I-131, exhibiting good in vitro stability. Subsequently, I-131-labeled PCMs are administered via the hepatic artery into rats with orthotopic HCC, leading to a significant increase in median overall survival (p < 0.05). Single photon emission computed tomography (SPECT/CT) imaging and immunohistochemical assessments demonstrate precise biodistribution and stable retention of I-131-PCMs in the liver for up to 14 days. Magnetic resonance imaging (MRI) further reveals the inhibition of tumor growth following I-131-PCM treatment. In summary, the I-131-PCMs display high radiolabeling efficiency, stability, and a promising radioembolization effect in the orthotopic HCC rodent model, highlighting their potential for use in interventional cancer therapy.

关键词： Radioembolization Microspheres Hepatocellular carcinoma Iodine-131

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Optimizing the miscibility for enhanced photovoltaic performance of non-fused ring electron acceptors through side-chain engineering

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS 2025年第13期27卷 6663-6668页

作者： Bai, Yahui Xie, linwei lin, Zhihui Ai, Qi Zhao, fuwen He, Dan Cent South Univ Coll Chem & Chem Engn State Key Lab Powder Met Changsha 410083 Peoples R China

Non-fused ring electron acceptors (NFREAs), notable for their simple and economical synthesis processes, play a pivotal role in the practical deployment of organic solar cells (OSCs). However, the power conversion efficiency (PCE) of NFREA based devices lags behind that of fused ring electron acceptors, because of the inferior charge transport and severe charge recombination in donor:NFREA blend films. In this study, we synthesized two novel NFREAs, A1C4-Cl and A1C6-Cl, featuring different alkyl side-chain lengths to optimize the miscibility between the donor and NFREAs for ideal morphology, taking into consideration that the morphology of donor:NFREA blend films has a significant influence on charge transport and recombination. The PBDB-T:A1C6-Cl based OSC exhibits better miscibility and more favourable phase separation, resulting in enhanced charge carrier mobilities and suppressed trap-assisted recombination. These improvements lead to a significant increase in short-circuit current density (JSC) and fill factor (FF), culminating in a PCE of 12.11% compared to PBDB-T:A1C4-Cl based devices. Our findings offer an effective approach to modulate the miscibility between donors and NFREAs, thereby enhancing the PCE of OSCs through the fine-tuning of alkyl side-chain lengths.

关键词： Organic solar cells

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Does transurethral resection of the prostate before robot-assisted radical prostatectomy have adverse effects on patients diagnosed with prostate cancer: a comparative evidence-based analysis?

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JOURNAL OF ROBOTIC SURGERY 2025年第1期19卷 1-16页

作者： Hu, Anneng lin, Yuhang Zhu, Xiaole Li, Junyang Luo, fuwen Yu, Xiaodong North Sichuan Med Coll Affiliated Hosp Dept Urol 1 Mao Yuan South Rd Nanchong 637000 Sichuan Peoples R China

In clinical practice, it is not uncommon for a history of trans-urethral resection of the prostate (TURP) to complicate a future robotic-assisted radical prostatectomy (RARP). This study aims to determine if prior TURP adversely affects outcomes in subsequent RARP, analyzing perioperative, functional, and oncological results between the procedures. Research published in English before September 2024 was systematically reviewed using Web of Science, PubMed, Cochrane Library, and the EMBASE. Review Manager 5.4 was used to do the meta-analysis, included 15 studies, with 869 patients who underwent RARP following TURP and 5,879 patients who underwent RARP alone. Compared to standard RARP, RARP following TURP was associated with extended operative time (OT) (WMD: 26.63 min, 95% CI: 16.79-36.48, P < 0.00001), increased estimated blood loss (EBL) (WMD: 19.85 ml, 95% CI: 9.22-30.48, P = 0.0003), longer hospital stay(LOS) (WMD: 0.52 days, 95% CI: 0.28-0.77, P < 0.0001), and extended catheter removal duration (WMD: 0.18 days, 95% CI: 0.02-0.35, P = 0.03). The overall nerve-sparing success rate was lower (OR: 0.53, 95% CI: 0.35-0.78, P = 0.001), with reduced bilateral nerve-sparing success rates (OR: 0.58, 95% CI: 0.39-0.84, P = 0.005). Patients in the TURP group had higher rates of bladder neck reconstruction (OR: 8.38, 95% CI: 5.80-12.10, P < 0.0001) and major complications (Clavien grade >= 3) (OR: 1.94, 95% CI: 1.10-3.41, P = 0.02). Furthermore, the positive surgical margin (PSM) rate was elevated in the prior-TURP group (OR: 1.25, 95% CI: 1.02-1.53, P = 0.03). Quality-of-life outcomes indicated that patients undergoing RARP after TURP experienced lower urinary incontinence recovery rates at one year (OR: 0.58, 95% CI: 0.34-0.97, P = 0.04) and reduced continence recovery rates (OR: 0.60, 95% CI: 0.44-0.81, P = 0.007). Nevertheless, there were no notable differences between the two groups in terms of the rates of transfusions, unilateral nerve-sparing, lymphadenectomy, minor

关键词： Robotic-assisted radical prostatectomy (RARP) Transurethral resection of the prostate (TURP) Prostate cancer (PCa) functional and oncological outcomes Meta-analysis

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