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

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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Effects of Ga addition on the microstructure and mechanical performance of Sn-58Bi based alloys and the solder joints

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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS 2024年第34期35卷 1-12页

作者： Li, Fusheng Xu, Lei chen, Mingze Zhang, fuwen Wang, Zhigang Liu, Xixue He, Huijun Beijing COMPO Adv Technol Co Ltd Beijing 101407 Peoples R China GRIPM Adv Mat Co Ltd Beijing 101407 Peoples R China

In the research, 0.5 wt. % Ga were added in Sn-58Bi solder to investigate the effect of Ga addition on the microstructure and mechanical performance of Sn-58Bi based solders and corresponding solder joints. Elemental analysis of Ga-bearing bulk solder confirms the existence of solid solution Ga in beta-Sn matrix and network alpha-Ga phase. The result of tensile test and post-test fracture surface analysis indicates that Ga addition improves the ultimate tensile strength, however, it depletes the plasticity by the precipitation of alpha-Ga phase with low melting point. With 0.5 wt. % Ga addition, the eutectic structure was much refined and the interfacial product changes from traditional scallop-like Cu6Sn5 layer to smooth Cu9Ga4 IMCs. In addition, the shear strength of Sn-58Bi solder joint was effectively improved by Ga addition due to the refinement strengthening of solder matrix and the improvement of interfacial IMC morphology. The shear fracture path changes from transgranular fracture in Cu6Sn5 layer to interfacial fracture between solder and Cu9Ga4 IMC layer.

关键词： Tensile testing

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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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Theranostic radionuclides labeled biodegradable microspheres for the treatment of hepatocellular carcinoma with radioembolization

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RADIATION PHYSICS AND CHEMISTRY 2025年 232卷

作者： Pang, fuwen Deng, Haihui Peng, Deti He, Jian Zhao, Weicheng Yu, Liqian chen, Tuantuan Xie, Zonggui Cai, Huawei chen, Bin Shenzhen Tradit Chinese Med Hosp Dept Intervent Radiol 1 Fuhua Rd Shenzhen 518033 Peoples R China Shenzhen Tradit Chinese Med Hosp Dept Liver Dis Shenzhen 518033 Peoples R China West China Hosp Dept Nucl Med 37 Guoxue Alley Chengdu 610041 Peoples R China

Liver cancer, predominantly hepatocellular carcinoma (HCC), is the third leading cause of cancer-related deaths worldwide. Unfortunately, curative options like surgery and ablation are limited to 20% of cases due to the frequent diagnosis of HCC at intermediate or advanced stages. Taking advantage of the liver's dual blood supply, transarterial radioembolization (TARE) serves as a viable option when surgery is not possible. It entails the therapeutic intra-arterial injection of microspheres containing radioisotopes during hepatic embolization procedures. While TARE using Yttrium-90 (90Y) labeled resin or glass microspheres has demonstrated promising results in HCC treatment, challenges persist, including non-biodegradability impeding re-embolization, high density causing improper occlusion in capillaries, inherent imaging issues, and high costs. Within the dynamic landscape of advancing research in HCC treatment, this article aims to deliver a thorough review of biodegradable microspheres labeled with theranostic radionuclides in the clinical setting for HCC and addresses new developments, presenting the most relevant findings.

关键词： Hepatocellular carcinoma Transarterial radioembolization Theranostic radionuclides Biodegradable microspheres

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Ti6Al4V-0.55Fe合金连续升温过程的相变研究

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稀有金属材料与工程 2019年第12期48卷 3917-3923页

作者：汪常亮李峰陈福文常辉周廉南京工业大学

通过连续升温热膨胀法(DIL)研究了Ti6Al4V-0.55Fe合金在连续升温过程中的α相回溶(α+β→β)的热膨胀行为和显微组织演化。采用了1、5、10、15 K/min的4种升温速率对Ti6Al4V-0.55Fe合金进行热膨胀实验,结果发现:不同升温速率的α相回... 详细信息

通过连续升温热膨胀法(DIL)研究了Ti6Al4V-0.55Fe合金在连续升温过程中的α相回溶(α+β→β)的热膨胀行为和显微组织演化。采用了1、5、10、15 K/min的4种升温速率对Ti6Al4V-0.55Fe合金进行热膨胀实验,结果发现:不同升温速率的α相回溶曲线都展现出典型的“S”型曲线,表明α相回溶是一种由形核长大控制的过程。通过Kissinger-Akahira-Sunose(KAS)方法和Kolmogorov-Johnson-Mehl-Avrami(KJMA)模型分别得到α相回溶转变平均相变激活能E和随着α相回溶体积的增大所对应的Avrami指数n,可分为3个阶段,即相变初期(0

关键词： Ti6Al4V-0.55Fe 连续升温相变组织演化

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Surface hydroxyl-modulation for constructing isolated vanadium active species for propane dehydrogenation

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JOURNAL OF COLLOID AND INTERFACE SCIENCE 2025年 688卷 193-203页

作者： Yang, fuwen Zhang, Jie chen, Jinwei Wang, Gang Yu, Tong Li, Qian Shi, Zongbo Zhuo, Runsheng Wang, Ruilin Sichuan Univ Coll Mat Sci & Engn Chengdu 610065 Peoples R China Sichuan Univ Engn Res Ctr Alternat Energy Mat & Devices Minist Educ Chengdu 610065 Peoples R China REZEL Catalysts Corp Shanghai 200120 Peoples R China

Vanadium-based catalysts have been regarded as a promising candidate for Pt- and Cr-based materials in propane dehydrogenation (PDH) application. However, regulating the coordination environment and polymeric degree of vanadium oxides (VOX) at nanoscale level remains great challenges. Herein, an efficient VOX catalyst with the adjustable polymeric degree is achieved by a surface hydroxyl-modulation. Specially, the physicochemical properties of VOX species are precisely regulated by controlling the density and dispersion of hydroxyl (OH) on silicalite-1 (S-1). The properly introduced OH could effectively tailor the polymeric degree of VOX species. Characterization results reveal the VOX sites preferentially tend to migrate and anchor on the OH groups, thereby contributing to the high dispersion of VOX sites with tetrahedrally coordinated VO4 sites. Besides, the OH regulation is also favorable for moderating the surface V density, electron-rich V3+, and the isolated VOX active species. Benefiting from the active sites with suitable polymeric degree, the optimal 5VOX/S-1_550 catalyst exhibits outstanding catalytic activity (initial propane conversion of 24.5 %, initial propylene selectivity of 96.7 %) and stability under industrial conditions, which is comparable to the previously reported vanadium-based catalysts. This work not only affords an alternative methodology for the rational design of VOX-based catalysts, but also paves a way to improving PDH performance at the nanoscale.

关键词： Surface hydroxyl Vanadium oxides Structure-activity relationship Propane dehydrogenation Propylene production

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Regulation of Maleic Anhydride Selectivity for n-Butane Oxidation by Sb2O3-Modified Vanadium Phosphorus Oxide Catalysts

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 2024年第26期63卷 11392-11403页

作者： Zhao, Junyu Zhang, Jie Yang, fuwen Yu, Tong Li, Qian chen, Jinwei Wang, Gang Wang, Ruilin Sichuan Univ Coll Mat Sci & Engn Chengdu 610065 Peoples R China Sichuan Univ Engn Res Ctr Alternat Energy Mat & Devices Minist Educ Chengdu 610065 Peoples R China

Maleic anhydride (MA) is a significant chemical raw material to produce industrial products. Vanadium phosphorus oxide (VPO) catalyst is considered an excellent catalyst for the selective oxidation of n-butane to prepare MA. However, MA selectivity is still limited by the complex crystalline phases and morphological characteristics of VPO catalysts. Herein, orthorhombic Sb2O3 was proposed as a structural directing agent and electronic promoting agent to modify the VPO catalyst. The relationship between the structure and the catalytic performance was systematically investigated to reveal the effect of orthorhombic Sb2O3. Physical characterizations reveal the introduced orthorhombic Sb2O3 greatly contributes to improving the active phases and inhibiting the disadvantageous delta-VOPO4 phase. Besides, the active phase and surface chemical properties of the VPO catalyst are effectively regulated, which is beneficial to the selective oxidation of n-butane. As expected, the optimal 1Sb(2)O(3)-O@VPO catalyst demonstrates considerable n-butane conversion, MA selectivity, and MA yield. This work should open a feasible way to prepare efficient VPO catalysts for industrial catalysis.

关键词： Catalysts Crystals Oxidation Precursors Selectivity

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CALPHAD assessment of bio-oriented Ti-Zr-Sn system and experimental validation in Ti/Zr-rich alloys

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CALPHAD-COMPUTER COUPLING OF PHASE DIAGRAMS AND THERMOCHEMISTRY 2019年 67卷 101686-000页

作者： Tan, Junyi Xu, Guanglong Tao, Xiaoma chen, fuwen Cui, Yuwen Zhou, Lian Nanjing Tech Univ Tech Inst Adv Mat Nanjing 211816 Jiangsu Peoples R China Nanjing Tech Univ Coll Mat Sci & Engn Nanjing 211816 Jiangsu Peoples R China Guangxi Univ Sch Phys Sci & Technol Nanning 530004 Peoples R China

The development of CALPHAD-type thermodynamic database for Ti or Zr based biomedical alloys has been spurred by the increased interest in efficiently tailoring an alloy composition to obtain high stability of beta_bcc, low Young's modulus, and free of detrimental phases. However, the thermodynamic prediction is not adequate to be performed without the information of key sub-ternary Ti-Zr-Sn system. In present work, the thermodynamic assessment of Ti-Zr-Sn system is performed via a critical evaluation of phase equilibria and microstructure development in this ternary system. The partial isothermal sections at 1323 K and 1473 K with Sn content below 40 at. % are obtained by analyzing chemical compositions and crystal structures of individual phases in the annealed alloys. The composition homogeneity range of most phases is validated to favor a ternary extension paralleling to the Ti-Zr axis. Particularly, beta_bcc and eta phases (with the chemical composition (Ti, Zr)(5)Sn3+x) show complete solubility of Ti and Zr from Ti-Sn edge to Zr-Sn edge. With the database, negligible ternary solubility of Zr4Sn phase, microstructure development in the as-cast samples, and the controversial conclusions in literature are discussed. Most of the experimental findings, including equilibrium phase constitution, solidification sequence, DSC signals, projections of liquidus, are reproduced in a self-consistent way. The work moves towards the completeness of multi-component Ti/Zr thermodynamic database. It can be used for composition design of novel metastable beta-type biomedical alloys.

关键词： Ti-Zr-Sn Phase equilibria CALPHAD Thermodynamics Solidification

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Genomic insights into marine environment adaptation and conservation of the threatened olive ridley turtle ( Lepidochelys olivacea)

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ISCIENCE 2025年第2期28卷 111776页

作者： Yang, Lin chen, Yiting Wang, Shaofeng Zhang, chenglong Huang, Xin Du, Xin Zhou, Wenliang Wei, fuwen Southern Marine Sci & Engn Guangdong Lab Guangzhou Ctr Evolut & Conservat Biol Guangzhou Peoples R China Jiangxi Agr Univ Coll Forestry Jiangxi Key Lab Conservat Biol Nanchang 330045 Jiangxi Peoples R China Hong Kong Univ Sci & Technol Dept Ocean Sci Hong Kong Peoples R China Guangdong Huidong Sea Turtle Natl Nat Reserve Huizhou Peoples R China Marine Protected Area Adm Sansha City Hainan Peoples R China Chinese Acad Sci Inst Zool CAS Key Lab Anim Ecol & Conservat Biol Beijing 100101 Peoples R China

Sea turtles are marine flagship species and most of them are currently in a threatened state. Long-term surviving in the ocean has driven significant morphological and physiological changes for this group, which makes them an ideal model for studying adaptive evolution of marine environments. Herein, we present a chromosome-scale genome of Lepidochelys olivacea with a genome size of 2.22 Gb and a contig N50 of 97.3 Mb. Comparative genomic analyses uncovered a suite of adaptive changes in genes related to olfaction, vision, virus defense, and longevity, which may help explain the genetic underpinnings of its marine environment adaptation. We also observed that the genome-wide heterozygosity of L. olivacea was low (6.45e-4), consistent with its prolonged population decline. Overall, our study provides valuable genetic resources for understanding evolutionary adaptations to aquatic environment and for the conservation of this threatened species.

关键词： Evolutionary biology Genomics Nature conservation

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