Materials Chemistry Frontiers最新文献

{"title":"Flexible TADF-based organic X-ray scintillating films for high-resolution imaging†","authors":"Haoqiang Xu, Wenjing Zhao, Xinning Zhang, Jingjing Cui, Zhenhua Wang, Xiaowang Liu, Junqing Shi and Lei Ji","doi":"10.1039/D4QM00795F","DOIUrl":"https://doi.org/10.1039/D4QM00795F","url":null,"abstract":"<p >X-ray scintillators are commonly used, with significant applications in scientific research and daily life. However, most commercial scintillators are based on expensive mechanically rigid inorganic crystalline arrays, which normally bear a long-lived afterglow that reduces the resolution in dynamic X-ray monitoring, while low X-ray absorbance and inefficient exciton utilization are deficiencies associated with traditional organic scintillators. Herein, we report a series of readily obtained pure organic single-component scintillators with halogen-enhanced X-ray absorbance, high fluorescence quantum yield, and short decay time. They can be easily prepared into flexible and transparent scintillating imaging films with a high light yield (approaching 20 000 photons MeV<small>⁻¹</small>) and high resolution (above 20 line pairs per mm) that are among the highest levels for organic scintillators reported thus far.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 3","pages":" 480-486"},"PeriodicalIF":6.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107456","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Nanogenerators with l-arginine loading: new choices as cascade and synergistic nitric oxide/photodynamic antitumor agents","authors":"Yue Huang, Ziwei Wu, Hanyang Wang, Hao An, Jiabao Zhang and Zhihong Bao","doi":"10.1039/D4QM00851K","DOIUrl":"https://doi.org/10.1039/D4QM00851K","url":null,"abstract":"<p >Photodynamic therapy (PDT) is widely used in tumor treatment because it has few side effects and good therapeutic specificity. However, its therapeutic effect is severely limited by the insufficient oxygen supply and high glutathione (GSH) concentration in the tumor environment. Recently, nitric oxide (NO) has been widely used as a physiological regulatory factor and tumor inhibitor in various pathological processes. NO can kill tumor cells by reacting with O<small>₂</small>˙<small>⁻</small> to produce highly lethal ONOO<small>⁻</small>. Importantly, NO can promote vasodilation to improve hypoxia in the tumor environment and interfere with the antioxidant defense of GSH, improve the sensitivity of the tumor to ROS, and enhance the effect of PDT. However, since NO has a very short half-life and is gaseous, it cannot be used directly in the clinic. As a rule, the use of NO donors is required. <small>L</small>-Arginine (<small>L</small>-Arg) is a natural NO donor that can produce NO under the action of ROS, so that effective synergy of NO/PDT can be achieved by combining <small>L</small>-Arg and a photosensitizer. On this basis, cascade and synergistic NO/PDT antitumor therapy with <small>L</small>-Arg has been reported in recent years. However, a relevant review on cascade and synergistic NO/PDT based on the combination of <small>L</small>-Arg and photosensitizers has not been published. Therefore, in this review, we summarize the recent advances in synergistic NO/PDT for antitumor therapy based on the interaction of <small>L</small>-Arg and various photosensitizers in the last five years. The design idea, synergistic mechanism and application prospects of the two treatment methods are explained in detail. The remaining challenges and future opportunities in this field are also highlighted. We believe that this review will provide a better understanding of cascade and synergistic NO/PDT through multifunctional nanomaterials and advance nanoscience and nanotechnology step by step towards clinical applications.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 204-222"},"PeriodicalIF":6.0,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Constructing vertically aligned ZIF-67 microrod arrays on carbon cloth with commercial-level mass-loading for high-performance supercapacitors†","authors":"Chenchen Bai, Bingjun Li, Dejun Li, Yan Han and Caiyun Wang","doi":"10.1039/D4QM00818A","DOIUrl":"https://doi.org/10.1039/D4QM00818A","url":null,"abstract":"<p >A facile solution immersion was developed to construct three-dimensional (3D) vertically aligned zeolite imidazole framework ZIF-67 microrod arrays on 3D carbon cloth (CC) with commercial-level mass loading (12 mg cm<small>⁻²</small>). It was realized <em>via in situ</em> crystallization with the assistance of electrodeposited reactive cobalt layer and seed-oriented growth associated with a high concentration of Co<small>²⁺</small>. The as-obtained ZIF-67/CC hybrid featured a 3D/3D hetero-structure with easily accessible channels, abundant electroactive sites and highly conductive networks. As integrated electrodes for supercapacitors, they could achieve a high specific capacitance (3396 mF cm<small>⁻²</small> at 1 mA cm<small>⁻²</small>) with superior rate capability (91% at 10 mA cm<small>⁻²</small>) and long-term cyclic stability (over 99% after 10 000 cycles). Furthermore, the assembled asymmetrical supercapacitor delivered a maximum energy density of 380 mW h cm<small>⁻²</small> at a power density of 1600 mW cm<small>⁻²</small>. Such characteristics suggest that the well-aligned ZIF-67 arrays on CC substrate have enormous potential for use in high-performance supercapacitors and can serve as an important platform for other applications, such as energy storage, catalysis and gas adsorption/separation.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 3","pages":" 436-444"},"PeriodicalIF":6.0,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A hydrophilic-Zn2+ conductive lanthanum phosphate interlayer toward ultra-long-life Zn anodes and zinc ion capacitors†","authors":"Yuequn Li, Yanjie Wang, Zhe Fang, Shaopei Jia, Xukai Wu, Zhiheng Wang, Kunyang Geng, Kongyao Chen, Yunchao Mu, Lin Zhang and Liwei Mi","doi":"10.1039/D4QM00868E","DOIUrl":"https://doi.org/10.1039/D4QM00868E","url":null,"abstract":"<p >The detrimental interfacial side reactions and irregular Zn dendrites may reduce the cycling life of Zn anodes and Zn-based energy storage devices. Regulating the interfacial microenvironment to eliminate harmful side reactions and achieve uniform Zn deposition is vital to develop high-performance Zn anodes. Here, a “hydrophilic-Zn<small>²⁺</small> conductive” lanthanum phosphate (LaPO<small>₄</small>) interlayer is applied to realize an ultra-long-life Zn anode (LAP-Zn) and Zn<small>²⁺</small> capacitors. The hydrophilic LaPO<small>₄</small> can act as a microscopic “H<small>₂</small>O-reservoir” by preferentially adsorbing H<small>₂</small>O molecules (the adsorption energy of LaPO<small>₄</small>–H<small>₂</small>O is −1.17 eV, larger than that of Zn–H<small>₂</small>O). Consequently, a microscopic H<small>₂</small>O-poor environment on the Zn anode is formed, thus eliminating harmful side reactions including H<small>₂</small> evolution and Zn corrosion. Simultaneously, Zn<small>²⁺</small> de-solvation is promoted, facilitating accelerated interfacial migration and uniform flux of Zn<small>²⁺</small>. The Zn<small>²⁺</small> migration number of LAP-Zn is 0.84 which is higher than that of pure Zn, demonstrating excellent Zn<small>²⁺</small> conductivity. The LAP-Zn//LAP-Zn symmetrical cell operates efficiently for over 700 h at 5 mA cm<small>⁻²</small> and 2 mA cm<small>⁻²</small>. The LAP-Zn//activated carbon capacitor exhibits an ultra-long life of 30 000 cycles at 1 A g<small>⁻¹</small>, with continuous operation for over 3600 h while maintaining a capacity retention ratio of 95%. Therefore, this “hydrophilic-Zn<small>²⁺</small> conductive” LaPO<small>₄</small> interlayer enables uniform Zn deposition and a highly reversible Zn plating/stripping process. This modification strategy using a “hydrophilic-Zn<small>²⁺</small> conductive” rare earth-based interfacial layer is simple, long-term effective, and microcosmic, thus boosting the commercial application of Zn-based energy storage devices.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 299-307"},"PeriodicalIF":6.0,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976289","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structural modulation of NH4V4O10 cathode materials for low-temperature zinc-ion energy-storage devices","authors":"Yaotong Li, Chunru Zhao, Wei Wang, Xiang Wu and Yudai Huang","doi":"10.1039/D4QM00890A","DOIUrl":"https://doi.org/10.1039/D4QM00890A","url":null,"abstract":"<p >With the characteristics of nontoxicity and environmental benignity, aqueous zinc ion batteries (AZIBs) are rapidly emerging as potential competitors for high-performance energy-storage systems. Nevertheless, several issues hinder their further development, such as the sluggish electrochemical activity and inevitable dissolution of cathode materials. In this work, we introduced oxygen defects (O<small>_d</small>) into the NH<small>₄</small>V<small>₄</small>O<small>₁₀</small> lattice, which facilitated the transport velocity of Zn<small>²⁺</small> ions and enhanced their electrical conductivity. Zn//NHVO-O<small>_d</small>-1 batteries showed a reversible capacity of 475.3 mA h g<small>⁻¹</small> at 0.2 A g<small>⁻¹</small>. At low temperature (0 °C), the cells also demonstrated a capacity retention of 100% after 1000 cycles at 1.0 A g<small>⁻¹</small>. Assembled soft-package devices presented favorable mechanical resilience at different bending conditions.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 243-252"},"PeriodicalIF":6.0,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976261","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Application and development of SERS technology in detection of VOC gases","authors":"Xiangyu Meng, Yuening Wang, Xiaoyu Song, Yue Liu, Yujiao Xie, Lei Xu, Jian Yu, Lin Qiu, Xiaotian Wang and Jie Lin","doi":"10.1039/D4QM00812J","DOIUrl":"https://doi.org/10.1039/D4QM00812J","url":null,"abstract":"<p >Volatile organic compounds (VOCs), are recognized as critical environmental contaminants and cancer biomarkers, highlighting the significance of their trace detection for environmental conservation and human health. Surface-enhanced Raman spectroscopy (SERS) technology has emerged as a promising tool in this domain, offering unparalleled sensitivity and the ability to provide molecular fingerprints for probes. Despite the inherent disadvantages of gaseous molecules being difficult to adsorb on solid substrates, researchers have made great efforts to overcome these obstacles. This comprehensive review delineates the recent advancements and applications of SERS technology in the detection of VOCs, encompassing environmental monitoring and the analysis of exhaled breath. A particular focus is placed on the innovative design of substrate materials and strategies for enhancing the capture of gas molecules, including metal–organic frameworks (MOFs), layered double hydroxides (LDHs), microfluidic chips, and other substrates. Finally, we summarized the current challenges confronting SERS technology in VOC detection and provided insights into potential prospects for future development.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 3","pages":" 349-366"},"PeriodicalIF":6.0,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Exogenous/endogenous stimuli-responsive nanocatalysts trigger in situ chemical reactions for tumor catalytic therapy: an up-to-date mini-review","authors":"Kaiyue Song, Cong Jiang, Shaorong Huang and Xianglong Li","doi":"10.1039/D4QM00833B","DOIUrl":"https://doi.org/10.1039/D4QM00833B","url":null,"abstract":"<p >The principle of the nanocatalytic medicine strategy is introducing nanocatalysts into tumor tissues and triggering specific chemical reactions through endogenous/exogenous stimuli to convert low/non-toxic exogenously delivered or endogenous substances into therapeutic products with high cytotoxicity. In recent years, the nanocatalytic medicine strategy has been proven to be effective in achieving tumor catalytic therapy, which is expected to reduce side effects and decrease the occurrence of drug resistance. This mini-review briefly outlines typical applications and recent advances in nanocatalyst-triggered <em>in situ</em> chemical reactions in tumor catalytic therapy. Special attention is paid to the design of nanocatalysts related to endogenous and exogenous stimuli (<em>e.g.</em>, light, heat, ultrasound, <em>etc.</em>). Finally, challenges and future opportunities for advancing nanocatalysts are highlighted to facilitate the realization of early clinical applications of nanocatalytic medicine strategies.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 189-203"},"PeriodicalIF":6.0,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pyrene-based, red-emitting, aggregation-induced emission luminogens: from structural construction to anti-counterfeiting applications†","authors":"Hua-Long Li, Zeng-Min Xue, Guang Yang, Fei Meng, Hong-Tao Lin, Wen-Xuan Zhao, Shu-Hai Chen and Chuan-Zeng Wang","doi":"10.1039/D4QM00927D","DOIUrl":"https://doi.org/10.1039/D4QM00927D","url":null,"abstract":"<p >Herein, we demonstrated a novel approach to construct pyrene-based, high-efficiency, red-emitting molecules. Both of the as-synthesized luminogens exhibited aggregation-induced enhanced emission (AIEE) properties and distinct mechanochromic behavior with a blue-shift for <strong>DCI-Py-1</strong> (13 nm) and red-shift for <strong>DCI-Py-2</strong> (29 nm). The typical, yet rare, pyrene-based, red-emitting molecules with <em>λ</em><small>_em</small> = 686 nm open up new avenues to design near-infrared emitting pyrene-based photoelectric materials. Further studies revealed that both of these materials can be utilized for anti-counterfeiting stamps and fingerprint extraction.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 318-324"},"PeriodicalIF":6.0,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976291","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Near-infrared II photochromic behavior triggered by green light in an in situ protonated dithienylethene functionalized by quinoxalinone moieties†","authors":"Ziyong Li, Jinzhao Song, Qilian Wang, Yongliang Feng, Qingxin Song, Sixin Wang, Qianqian Nie, Fan He, Haining Zhang and Hui Guo","doi":"10.1039/D4QM00719K","DOIUrl":"https://doi.org/10.1039/D4QM00719K","url":null,"abstract":"<p >Exploiting the near-infrared (NIR) photochromic dithienylethenes (DTEs) triggered by visible light is urgently needed for various biological scenarios. However, all the NIR photochromic DTEs reported so far are located in the first NIR window (NIR-I, 700–900 nm), which usually shows shallower penetration in biological tissues due to autofluorescence and photon scattering compared to NIR light in the second window (NIR-II, 1000–1700 nm). Herein, we present a novel quinoxalinone-functionalized DTE derivative (<strong>QDTE</strong>) with acceptor (A)–DTE (D)–acceptor (A) structural features, in which electron-withdrawing quinoxalinone groups ensure visible light-driven NIR I photochromism. Besides, the facile protonation of the quinoxalinone moieties favors the formation of the more electron-deficient A′–D–A′-type DTE (<strong>QDTE-2H</strong>, where A′ is a stronger electron-withdrawing unit) for a unique NIR II photochromism by reducing the HOMO–LUMO energy gap of a closed isomer after protonation. As expected, the resulting <strong>QDTE</strong> displays a blue light-controlled NIR I photochromic performance in various solvents. Furthermore, an unprecedented green light-triggered NIR II photochromism for the <em>in situ</em> protonated <strong>QDTE-2H</strong> is successfully implemented in CHCl<small>₃</small> and toluene in the presence of trifluoroacetic acid (TFA), representing the first case of NIR II photochromic DTE. By virtue of these properties, <strong>QDTE</strong> has been successfully applied in dual information encryption, demonstrating its versatility in functional materials.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 234-242"},"PeriodicalIF":6.0,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976260","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic enhancement of the electrocatalytic reduction of CO2 to hydrocarbons at a large-sized Cu@Ag electrode†","authors":"Ke-Ke Chang, Wan-Feng Xiong, Yu-Ting Wen, Bin-Bin Feng, Hong-Fang Li, Teng Zhang, Yuan-Biao Huang, Duan-Hui Si and Rong Cao","doi":"10.1039/D4QM00819G","DOIUrl":"https://doi.org/10.1039/D4QM00819G","url":null,"abstract":"<p >The electrochemical CO<small>₂</small> reduction reaction (CO<small>₂</small>RR) underlies a strategic approach to energy and environmental challenges. Large-sized materials offer industrial scalability due to their simplicity and cost-effectiveness. However, traditional large-sized Cu catalysts preferentially catalyze the hydrogen evolution reaction (HER) over the CO<small>₂</small>RR. Hence, the development of large-sized catalysts with enhanced reducibility is imperative for an efficient CO<small>₂</small>RR. In this study, a large-sized Cu@Ag catalyst was designed using electrodeposition, which enhanced the CO<small>₂</small>RR and suppressed the HER. The faradaic efficiency (FE) for hydrocarbons of the Cu@Ag catalyst was 59.8%, surpassing that of bare Cu nanoparticles by 21.4%. FE<small>_{H<small>₂</small>}</small> was notably reduced to 31.6%, compared to 63.0% for Ag foil and 55.2% for bare Cu nanoparticles. Theoretical calculations indicated a reconfiguration of Cu 3d orbitals in the Cu@Ag catalyst. The d<small>_{<em>x</em><small>²</small>−<em>y</em><small>²</small>}</small> orbital, being the highest occupied, modulated the affinity of CO<small>₂</small> molecules and favored hydrocarbon formation. Additionally, the charge density at the Cu@Ag boundaries increased, facilitating C–C coupling. In particular, the C<small>₂</small>H<small>₄</small>/CH<small>₄</small> ratio was enhanced by approximately 30-fold compared to using bare Cu nanoparticles. This study demonstrated that the synergistic mechanism of the Cu@Ag catalyst is key to enhancing the CO<small>₂</small>RR and inhibiting the competing HER, thus elucidating the molecular mechanisms for the conversion of CO<small>₂</small> into valuable chemicals using large-sized Cu-based catalysts.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 2","pages":" 271-279"},"PeriodicalIF":6.0,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}