Mengling Yang, Chunyu Wang, Wenbin Wang, Li Yang, Shaolei Qu, Zhaoming Zhang and Xuzhou Yan
{"title":"Multiple hydrogen bonding in crosslinked graphene oxide films with improved stretchability and toughness†","authors":"Mengling Yang, Chunyu Wang, Wenbin Wang, Li Yang, Shaolei Qu, Zhaoming Zhang and Xuzhou Yan","doi":"10.1039/D4QM00571F","DOIUrl":"10.1039/D4QM00571F","url":null,"abstract":"<p >Transforming the microscopic graphene oxide (GO) nanosheets into macroscopic film materials holds significant promise for various applications. However, those GO films normally suffer from low tensile strength and poor toughness. Optimizing the assembly of GO nanosheets, especially in designing the interactions between adjacent nanosheets, remains challenging. Herein, inspired by mussels, we incorporated polymer rich in UPy functional units into GO films, namely GUPy films. The multiple hydrogen bonding between the UPy units and oxygen-containing groups on GO nanosheets resulted in highly stretchable and tough GO films. Scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) confirmed the presence of UPy in the films, revealing tightly linked layered structures at the microscopic level. Macroscopically, the films displayed exceptional flexibility, withstanding folding and curling without damage. Tensile tests demonstrated the superior mechanical properties of the GUPy film, which boasts a Young's modulus of 1100.5 MPa, fracture strain of 24.0%, tensile strength of 183.5 MPa, and toughness of 19.5 MJ m<small><sup>−3</sup></small>. These values are 2.3, 2.4, 6.0, and 12.2 times higher than those of pure GO films, respectively, and significantly exceed those of control films lacking UPy. Additionally, cyclic tensile tests confirmed the excellent energy dissipation capability of the GUPy film. This bio-inspired strategy offers a promising route for developing high-performance two-dimensional materials, expanding their potential applications.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 22","pages":" 3724-3730"},"PeriodicalIF":6.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202612","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}
Yu Jiang, Yuqing Li, Qunting Qu, Linze Lv, Jie Shao, Jing Wang and Honghe Zheng
{"title":"Reuse of spent industrial graphite in batteries by green recycling and interphase functionalization†","authors":"Yu Jiang, Yuqing Li, Qunting Qu, Linze Lv, Jie Shao, Jing Wang and Honghe Zheng","doi":"10.1039/D4QM00438H","DOIUrl":"10.1039/D4QM00438H","url":null,"abstract":"<p >With the widespread application of Li-ion batteries (LIBs) and the attendant appearance of large amounts of spent LIBs, recycling discarded graphite anodes is of great significance from the perspective of saving energy and resource sustainability. The conventional strategies for recycling graphite mainly include strong acid leaching and high-temperature calcination, which are environmentally hazardous or energy consuming. This work develops a green, economical and effective method to recover graphite from spent LIBs, which involves low-concentration organic citric acid leaching and a subsequent gravity separation process with a gelatin solution. This recycling route can increase the safety and operational feasibility of the industry, save energy, and thoroughly remove the metal-based and lightweight carbon-based impurities. Meanwhile, the graphite surface is functionalized with a gelatin layer, which works as an artificial interphase, suppresses electrolyte decomposition, and protects the graphite structure. The recycled graphite is further used as the cathode material in high-voltage (5.0 V) dual-ion batteries, exhibiting rapid charge/discharge capability and excellent cycling stability with a capacity retention of 87.9% after 4500 cycles. This work will be of great significance for the recycling of graphite and the sustainable development of energy storage technologies.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3653-3663"},"PeriodicalIF":6.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202700","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}
Jiajun Gong, Zhicheng Yao, Qimin Peng, Huizi Tang, Wenhao Han and Shimou Chen
{"title":"Dissociating high concentration lithium salts in LLZTO-based high dielectric polymer electrolytes for low temperature Li metal batteries†","authors":"Jiajun Gong, Zhicheng Yao, Qimin Peng, Huizi Tang, Wenhao Han and Shimou Chen","doi":"10.1039/D4QM00625A","DOIUrl":"10.1039/D4QM00625A","url":null,"abstract":"<p >Incorporating high concentrations of lithium salts into solid polymer electrolytes can enhance the electrochemical performance of Li metal batteries. However, this approach is often obstructed by the reduced mechanical properties and limited lithium salt dissociation capacity. To address these challenges, we coupled a rigid inorganic solid electrolyte, Li<small><sub>6.4</sub></small>La<small><sub>3</sub></small>Zr<small><sub>1.4</sub></small>Ta<small><sub>0.6</sub></small>O<small><sub>12</sub></small> (LLZTO), with a high-dielectric-constant polymer, polyvinylidene-trifluoroethylene-trifluoroethylene chloride. The resulting composite solid electrolyte (named PTCL-1.5) significantly improves Li<small><sup>+</sup></small> transport at low temperatures. The assembled Li|PTCL-1.5|Li cell demonstrates remarkable cycling stability, operating for over 4350 hours at −20 °C and 0.1 mA cm<small><sup>−2</sup></small>. The PTCL-1.5 electrolyte exhibits excellent compatibility with various cathodes. Specifically, the Li|PTCL-1.5|LiNi<small><sub>0.8</sub></small>Co<small><sub>0.1</sub></small>Mn<small><sub>0.1</sub></small>O<small><sub>2</sub></small> cell achieves a capacity of 127.69 mA h g<small><sup>−1</sup></small> at −20 °C, while the Li|PTCL-1.5|LiFePO<small><sub>4</sub></small> cell shows exceptional cycle stability, exceeding 750 cycles. Our work offers a promising approach for developing solid-state electrolytes with high electrochemical stability at low temperatures.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3569-3576"},"PeriodicalIF":6.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202609","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":"Fabrication of closed-cell inverse opal photonic crystal pigments with angle-independent and stable structural colors†","authors":"Qianyao Fang, Shijia Wang, Jiahao Li and Xin Su","doi":"10.1039/D4QM00608A","DOIUrl":"10.1039/D4QM00608A","url":null,"abstract":"<p >Brilliant and non-photobleaching structural colors make photonic crystal (PC) pigments an appealing replacement for traditional chemical pigments. However, pigments with angle-independent structural colors are usually fabricated through amorphous arrays, PC balls or PC powders with an opal or inverse opal structure, which suffer from problems such as pale colors, inefficient and tedious fabrication processes as well as unstable indefinite colors during usage. Herein, PS@SiO<small><sub>2</sub></small> core–shell spheres were first synthesized and assembled into an opal template with SiO<small><sub>2</sub></small> sol infiltrated into interstices between the spheres. Subsequent calcination transformed PS cores into pores enclosing <em>in situ</em> formed carbon black. Thus, bulk closed-cell inverse opal PCs (IOPCs) were obtained with ordered and isolated pores embedded into a continuous SiO<small><sub>2</sub></small> matrix. After being ground into fine powders, PC pigments with three vivid and angle-independent primary structural colors were obtained with 268 nm, 305 nm and 352 nm PS@SiO<small><sub>2</sub></small> spheres as building blocks. The closed cells protect the pores from infiltration of the solvent inside and maintain the necessary refractive index between the pores and SiO<small><sub>2</sub></small> matrix for bright structural colors. Thus, PC pigments with stable colors can be mixed with linseed oil and painting medium to prepare painting pigments, which can be used for painting a delicate pattern with multiple colors. The stable, vivid and angle-independent structural colors and the abundant colors from the color mixing effect endow the PC pigments with great value in broad potential applications, including art, aesthetics and displays.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 22","pages":" 3731-3740"},"PeriodicalIF":6.0,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202636","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}
Junmei Li, Yinan Fan, Ruigan Zhang, Demao Ban, Zhixuan Duan, Xiaoyuan Liu and Lifang Liu
{"title":"A review on metal–organic frameworks (MOFs) and MOF–textile composites for personal protection","authors":"Junmei Li, Yinan Fan, Ruigan Zhang, Demao Ban, Zhixuan Duan, Xiaoyuan Liu and Lifang Liu","doi":"10.1039/D4QM00358F","DOIUrl":"10.1039/D4QM00358F","url":null,"abstract":"<p >Metal–organic frameworks (MOFs) have become a research hotspot for effective adsorption and degradation of chemical warfare agents (CWAs) and toxic industrial chemicals (TICs) due to their low density, large pore capacity, and customizable structure. However, their further development is seriously hampered by the low stability of MOFs and poor cycle durability. Personal protective equipment (PPE) is the focus of current research as the last barrier to protect people from harm. However, there are still gaps in related research, and the application of MOF–textile composites in personal protection is rarely reported. In this review, the relevant mechanisms of MOFs for the catalysis and adsorption of CWAs are briefly discussed, as well as the research status of MOF adsorption of TICs. Finally, the preparation of MOF–textile composites and their potential for personal protective equipment (PPE) are summarized, and the potential applications of MOFs in chemical protection are prospected.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3509-3527"},"PeriodicalIF":6.0,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202613","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}
Jiejie Ping, Mei Wu, Manyu Liu, Yan Jiang, Wenhui Shang, Menggai Jiao, Jiahao Ruan, Nan Wang and Zhiyu Jia
{"title":"Porphyrin-linked graphdiyne as a substrate for constructing single-atom catalysts with transition metals towards oxygen reduction reactions and oxygen evolution reactions†","authors":"Jiejie Ping, Mei Wu, Manyu Liu, Yan Jiang, Wenhui Shang, Menggai Jiao, Jiahao Ruan, Nan Wang and Zhiyu Jia","doi":"10.1039/D4QM00555D","DOIUrl":"10.1039/D4QM00555D","url":null,"abstract":"<p >Porphyrin-linked graphdiyne (PGDY) is a carbon-based material that provides a platform for anchoring single-atom catalysts (SACs) with transition metals (TMs). These SACs have the potential to boost the catalytic activity of the PGDY substrate. The synthesized TM@PGDY composites showed remarkable catalytic activity towards oxygen reduction reactions and oxygen evolution reactions.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 22","pages":" 3741-3746"},"PeriodicalIF":6.0,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202635","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}
Junjie Wang, Bo Wang, Xinmeng He, Jun Lv, Zhiyong Bao, Jiewu Cui, Guangqing Xu and Wangqiang Shen
{"title":"Nickel sulfide cocatalyst-modified silicon nanowire arrays for efficient seawater-based hydrogen generation†","authors":"Junjie Wang, Bo Wang, Xinmeng He, Jun Lv, Zhiyong Bao, Jiewu Cui, Guangqing Xu and Wangqiang Shen","doi":"10.1039/D4QM00366G","DOIUrl":"10.1039/D4QM00366G","url":null,"abstract":"<p >Silicon nanowire arrays (SiNWs) have shown considerable potential as water splitting materials because of their excellent light absorption ability and high surface area-to-volume ratio, which promote photoelectrochemical reactions. However, the catalytic activity of SiNWs for hydrogen evolution is hindered by the slow charge transfer kinetics. Herein, we propose a new approach to boost hydrogen production in simulated seawater employing NiS<small><sub><em>x</em></sub></small> cocatalyst-decorated SiNWs photocathodes. The integration of NiS<small><sub><em>x</em></sub></small> cocatalyst onto SiNWs considerably improves the catalytic performance, enabling efficient hydrogen evolution under simulated sunlight irradiation. The HER performance of NiS<small><sub><em>x</em></sub></small>/SiNWs photocathodes was systematically investigated in simulated seawater. The optimized photocathode exhibited an onset potential of 0.068 V <em>vs.</em> RHE while the SiNWs photocathode showed an onset potential at −0.597 V <em>vs.</em> RHE. Moreover, a remarkable hydrogen evolution rate of 189.15 μmol h<small><sup>−1</sup></small> cm<small><sup>−2</sup></small> was obtained, which is 30.86 times higher than that of pristine SiNWs. Systematic experimental investigations confirmed that the <em>in situ</em> grown nickel sulfide (NiS<small><sub><em>x</em></sub></small>) provides abundant active sites for HER with enhanced photoelectrochemical activity. Furthermore, a stable interface was constructed between SiNWs and NiS<small><sub><em>x</em></sub></small>, which acts as an efficient transport channel of photoelectrons, simultaneously enabling the NiS<small><sub><em>x</em></sub></small>/SiNWs heterostructure with good stability against the alkaline electrolyte-induced deactivation process of the silicon surface. These noteworthy advancements considerably elevate the HER performance of the photocathode. Our findings underscore the potential of this hybrid photocathode system for sustainable hydrogen production from abundant seawater resources.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3634-3642"},"PeriodicalIF":6.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202634","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":"Highly selective separation of toluene and methylcyclohexane based on nonporous adaptive crystals of hybrid[3]arene†","authors":"Shiqi Wei, Yuhao Wang and Jiong Zhou","doi":"10.1039/D4QM00590B","DOIUrl":"10.1039/D4QM00590B","url":null,"abstract":"<p >The efficient separation of toluene and methylcyclohexane is one of the biggest challenges in the field of chemical separation. Due to their closely matched boiling points, traditional distillation separation methods consume a lot of energy. Therefore, it is imperative to develop novel separation techniques to obtain toluene and methylcyclohexane with high purities. Herein, we develop an economical strategy for adsorptive separation based on nonporous adaptive crystals of hybrid[3]arene <strong>H</strong> (<strong>H<em>α</em></strong>). <strong>H<em>α</em></strong> selectively separate toluene from the mixture of toluene and methylcyclohexane (<em>v </em>:<em> v</em> = 1 : 1) with a purity of 100% <em>via</em> the vapor–solid adsorption and a purity of 98.98% <em>via</em> the liquid–solid adsorption. The selectivity arises from the stability of the new crystal structure after the capture of the preferred guest, toluene, by <strong>H<em>α</em></strong>. The reversible transition between guest-free and guest-loaded structures endows <strong>H<em>α</em></strong> with excellent recyclability.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 19","pages":" 3150-3156"},"PeriodicalIF":6.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202638","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}
Jiahao Li, Tongling Yu, Chengcai Wu, Qianyao Fang and Xin Su
{"title":"Coordination-bond-assisted fabrication of robust composite photonic crystal films through melt-compression†","authors":"Jiahao Li, Tongling Yu, Chengcai Wu, Qianyao Fang and Xin Su","doi":"10.1039/D4QM00566J","DOIUrl":"10.1039/D4QM00566J","url":null,"abstract":"<p >Embedding photonic crystals (PCs) into a polymer matrix and directly promoting the interactions between building blocks through various forces (such as coordination bonds) are effective strategies for fabricating robust PC films. However, owing to the adverse effect of metal salts on electrostatic repulsion during an assembly process, coordination bonds have long been ignored as an effective force for strengthening PC films. Herein, monodisperse PS@PEA-PAA core–shell spheres were prepared through a stepwise emulsion polymerization process, and a complex with ZnCl<small><sub>2</sub></small> to serve as a precursor for PC films was formed. Under vertical compression at elevated temperatures, polymer shell melt drove the assembly of PS cores into highly ordered arrays with steric repulsion as the necessary balancing force and locked the whole structure. With 1 mL of AA monomer added to PS@PEA-PAA building blocks and 2 mmol of ZnCl<small><sub>2</sub></small> added to form a complex precursor, compared with the results of PS@PEA PC films, coordination bonds in PS@PEA-PAA composite PC films induced a 420.8% increase in Young's modulus, which clearly demonstrates the impressive ability of coordination bonds to promote mechanical properties. Blue, green and red PC films were prepared as the basic elements using 225 nm, 265 nm and 310 nm PS@PEA-PAA spheres as building blocks, respectively, which can be further combined selectively into cyan, violet and yellow PC films following the additive color mixing rule. The robust free-stranding PC films can be further tailored and recombined into PC patterns with versatile designing styles and abundant optional structural colors, demonstrating great value for practical applications.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3624-3633"},"PeriodicalIF":6.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202640","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}
Xue Meng, Zhijun Wang, Xiaoxue Huo, Mingxin Zhou, Yu Wang and Panlai Li
{"title":"Novel high-efficiency near-infrared phosphor CaZrTaGaO7:Cr3+ and its application in night vision and anti-counterfeiting†","authors":"Xue Meng, Zhijun Wang, Xiaoxue Huo, Mingxin Zhou, Yu Wang and Panlai Li","doi":"10.1039/D4QM00558A","DOIUrl":"10.1039/D4QM00558A","url":null,"abstract":"<p >Near-infrared (NIR) light attracts attention because of its promising applications in night vision, anti-counterfeiting, biosensors, and measuring food composition and freshness. However, new NIR light sources with excellent thermal stability, higher efficiency, and superior photoelectric conversion efficiency are still a significant challenge. In this study, CaZrTaGaO<small><sub>7</sub></small>:0.01Cr<small><sup>3+</sup></small>, which can convert visible light into NIR light, was synthesized using a high-temperature solid-state method, and the crystal structure, morphology, site preference, and luminescence properties were investigated. Under 460 nm blue light excitation, the phosphor produces a broadband NIR emission in the 600–1100 nm region (<em>λ</em><small><sub>max</sub></small> = 829 nm), with a full width at half maximum of 178 nm, an internal quantum efficiency of 90.7%, and an excellent thermal stability of 84.8% at 423 K. A NIR light emitting diode (LED) was prepared using a 460 nm LED chip and CaZrTaGaO<small><sub>7</sub></small>:0.01Cr<small><sup>3+</sup></small>, and the new compound can produce strong NIR emission (273 mW at 100 mA) with a photoelectric conversion efficiency of 11.8%. Photographed phosphor-converted LEDs (pc-LEDs) with a regular camera and captured pc-LEDs in operation in the dark. The results indicate that this material may provide a new option for high power NIR night vision and other applications.</p>","PeriodicalId":86,"journal":{"name":"Materials Chemistry Frontiers","volume":" 21","pages":" 3608-3615"},"PeriodicalIF":6.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142202637","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}