Pub Date : 2024-09-28DOI: 10.1038/s43246-024-00638-6
Pankaj Bharmoria, Lukas Naimovičius, Deyaa Abol-Fotouh, Mila Miroshnichenko, Justas Lekavičius, Gabriele De Luca, Umair Saeed, Karolis Kazlauskas, Nicolas Candau, Paulius Baronas, Anna Roig, Kasper Moth-Poulsen
Biopolymers currently utilized as substitutes for synthetic polymers in photonics applications are predominantly confined to linear optical color responses. Herein we expand their applications in non-linear optics by integrating with triplet-triplet annihilation photon upconversion crystals. A photon upconverting biomaterial is prepared by cultivating Pd(II) meso-tetraphenyl tetrabenzoporphine: 9,10-diphenyl anthracene (sensitizer: annihilator) crystals on bacterial cellulose hydrogel that serves both as host and template for the crystallization of photon upconversion chromophores. Coating with gelatin improves the material’s optical transparency by adjusting the refractive indices. The prepared material shows an upconversion of 633 nm red light to 443 nm blue light, indicated by quadratic to linear dependence on excitation power density (non-linearly). Notably, components of this material are physically dis-assembled to retrieve 66 ± 1% of annihilator, at the end of life. Whereas, the residual clean biomass is subjected to biodegradation, showcasing the sustainability of the developed photonics material. Biopolymers used in photonics are mainly limited to linear optical color responses. Here, photon upconversion crystals incorporated into bacterial cellulose films demonstrate non-linear optical applications in biopolymers.
{"title":"Photon upconversion crystals doped bacterial cellulose composite films as recyclable photonic bioplastics","authors":"Pankaj Bharmoria, Lukas Naimovičius, Deyaa Abol-Fotouh, Mila Miroshnichenko, Justas Lekavičius, Gabriele De Luca, Umair Saeed, Karolis Kazlauskas, Nicolas Candau, Paulius Baronas, Anna Roig, Kasper Moth-Poulsen","doi":"10.1038/s43246-024-00638-6","DOIUrl":"10.1038/s43246-024-00638-6","url":null,"abstract":"Biopolymers currently utilized as substitutes for synthetic polymers in photonics applications are predominantly confined to linear optical color responses. Herein we expand their applications in non-linear optics by integrating with triplet-triplet annihilation photon upconversion crystals. A photon upconverting biomaterial is prepared by cultivating Pd(II) meso-tetraphenyl tetrabenzoporphine: 9,10-diphenyl anthracene (sensitizer: annihilator) crystals on bacterial cellulose hydrogel that serves both as host and template for the crystallization of photon upconversion chromophores. Coating with gelatin improves the material’s optical transparency by adjusting the refractive indices. The prepared material shows an upconversion of 633 nm red light to 443 nm blue light, indicated by quadratic to linear dependence on excitation power density (non-linearly). Notably, components of this material are physically dis-assembled to retrieve 66 ± 1% of annihilator, at the end of life. Whereas, the residual clean biomass is subjected to biodegradation, showcasing the sustainability of the developed photonics material. Biopolymers used in photonics are mainly limited to linear optical color responses. Here, photon upconversion crystals incorporated into bacterial cellulose films demonstrate non-linear optical applications in biopolymers.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00638-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-28DOI: 10.1038/s43246-024-00647-5
Estefani Marchiori, Giulio Romagnoli, Lukas Schneider, Boris Gross, Pardis Sahafi, Andrew Jordan, Raffi Budakian, Priya R. Baral, Arnaud Magrez, Jonathan S. White, Martino Poggio
Surfaces – by breaking bulk symmetries, introducing roughness, or hosting defects – can significantly influence magnetic order in magnetic materials. Determining their effect on the complex nanometer-scale phases present in certain non-centrosymmetric magnets is an outstanding problem requiring high-resolution magnetic microscopy. Here, we use scanning SQUID microscopy to image the surface of bulk Cu2OSeO3 at low temperature and in a magnetic field applied along $$leftlangle 100rightrangle$$ . Real-space maps measured as a function of applied field reveal the microscopic structure of the magnetic phases and their transitions. In low applied field, we observe a magnetic texture consistent with an in-plane stripe phase, pointing to the existence of a distinct surface state. In the low-temperature skyrmion phase, the surface is populated by clusters of disordered skyrmions, which emerge from rupturing domains of the tilted spiral phase. Furthermore, we displace individual skyrmions from their pinning sites by applying an electric potential to the scanning probe, thereby demonstrating local skyrmion control at the surface of a magnetoelectric insulator. Surfaces can significantly influence magnetic order by breaking bulk symmetries, introducing roughness, or hosting defects. Here, a microscopy study of the surface of bulk Cu2OSeO3 reveals magnetic textures associated with distinct surface states, such as in-plane magnetic stripes that are absent in the bulk, and demonstrates the local displacement of individual skyrmions by an applied electric field.
{"title":"Imaging magnetic spiral phases, skyrmion clusters, and skyrmion displacements at the surface of bulk Cu2OSeO3","authors":"Estefani Marchiori, Giulio Romagnoli, Lukas Schneider, Boris Gross, Pardis Sahafi, Andrew Jordan, Raffi Budakian, Priya R. Baral, Arnaud Magrez, Jonathan S. White, Martino Poggio","doi":"10.1038/s43246-024-00647-5","DOIUrl":"10.1038/s43246-024-00647-5","url":null,"abstract":"Surfaces – by breaking bulk symmetries, introducing roughness, or hosting defects – can significantly influence magnetic order in magnetic materials. Determining their effect on the complex nanometer-scale phases present in certain non-centrosymmetric magnets is an outstanding problem requiring high-resolution magnetic microscopy. Here, we use scanning SQUID microscopy to image the surface of bulk Cu2OSeO3 at low temperature and in a magnetic field applied along $$leftlangle 100rightrangle$$ . Real-space maps measured as a function of applied field reveal the microscopic structure of the magnetic phases and their transitions. In low applied field, we observe a magnetic texture consistent with an in-plane stripe phase, pointing to the existence of a distinct surface state. In the low-temperature skyrmion phase, the surface is populated by clusters of disordered skyrmions, which emerge from rupturing domains of the tilted spiral phase. Furthermore, we displace individual skyrmions from their pinning sites by applying an electric potential to the scanning probe, thereby demonstrating local skyrmion control at the surface of a magnetoelectric insulator. Surfaces can significantly influence magnetic order by breaking bulk symmetries, introducing roughness, or hosting defects. Here, a microscopy study of the surface of bulk Cu2OSeO3 reveals magnetic textures associated with distinct surface states, such as in-plane magnetic stripes that are absent in the bulk, and demonstrates the local displacement of individual skyrmions by an applied electric field.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00647-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Slot-die coating (SDC) technology is a potential approach to mass produce large-area, high-performance perovskite solar cells (PSCs) at low cost. However, when the interface in contact with the perovskite ink has low wettability, the SDC cannot form a uniform pinhole-free perovskite film, which reduces the performance of the PSC. To address this issue, in this study, the wettability of the hole transport layer (HTL) interface was investigated in depth by analyzing the variation of wettability with process and its correlation with the roughness of the HTL interface. As a result, it was found that SDC could increase the roughness of the HTL interface to improve wettability and form a uniform high-quality perovskite layer without pinholes, and furthermore, SDC-based NiOx/Me-4PACz HTL suppressed energy losses at the HTL/perovskite interface. In addition, a unit cell achieved 19.17% of efficiency with long-term stability and lab cell-sized modules showed up to 17.42%. Slot-die coating is promising for the large-scale and low-cost manufacture of perovskite solar cells. Here, the effect of wettability of the hole transport layer is investigated, finding that increased surface roughness improves wettability and prevents pinhole formation, favoring solar cell efficiency.
{"title":"Influence of interfacial roughness on slot-die coatings for scaling-up high-performance perovskite solar cells","authors":"Sushil Shivaji Sangale, Dilpreet Singh Mann, Hyun-Jung Lee, Sung-Nam Kwon, Seok-In Na","doi":"10.1038/s43246-024-00645-7","DOIUrl":"10.1038/s43246-024-00645-7","url":null,"abstract":"Slot-die coating (SDC) technology is a potential approach to mass produce large-area, high-performance perovskite solar cells (PSCs) at low cost. However, when the interface in contact with the perovskite ink has low wettability, the SDC cannot form a uniform pinhole-free perovskite film, which reduces the performance of the PSC. To address this issue, in this study, the wettability of the hole transport layer (HTL) interface was investigated in depth by analyzing the variation of wettability with process and its correlation with the roughness of the HTL interface. As a result, it was found that SDC could increase the roughness of the HTL interface to improve wettability and form a uniform high-quality perovskite layer without pinholes, and furthermore, SDC-based NiOx/Me-4PACz HTL suppressed energy losses at the HTL/perovskite interface. In addition, a unit cell achieved 19.17% of efficiency with long-term stability and lab cell-sized modules showed up to 17.42%. Slot-die coating is promising for the large-scale and low-cost manufacture of perovskite solar cells. Here, the effect of wettability of the hole transport layer is investigated, finding that increased surface roughness improves wettability and prevents pinhole formation, favoring solar cell efficiency.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00645-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-20DOI: 10.1038/s43246-024-00641-x
Yasmeen Shamiya, Aishik Chakraborty, Alap Ali Zahid, Nicholas Bainbridge, Jingyuan Guan, Biao Feng, Dominic Pjontek, Subrata Chakrabarti, Arghya Paul
Nanofiber-based hydrogel delivery systems have recently shown great potential in biomedical applications, specifically due to their high surface-to-volume ratio of ultra-fine nanofibers and their ability to carry low solubility drugs. Herein, we introduce a visible light-triggered in situ-gelling drug vehicle (GAP Gel) composed of ascorbyl palmitate (AP) nanofibers and gelatin methacryloyl polymer. AP nanofibers form self-assembled structures through intermolecular interactions with a hydrophobic drug-loading core. We demonstrate that the hydrophilic periphery of AP nanofibers allows them to interact with other hydrophilic molecules via hydrogen bonds. The presence of AP nanofibers significantly enhances the viscoelasticity of GAP Gel in a concentration-dependent manner. Further, GAP Gel shows in vitro biocompatibility and sustained drug delivery efficacy when loaded with a hydrophobic antibiotic. Likewise, GAP Gel shows excellent in vivo biocompatibility when implanted in immunocompetent mice in various forms. Lastly, GAP Gels maintain cell viability when cultured in a 3D-environment over 7 days, establishing it as a promising and versatile hydrogel platform for the delivery of biotherapeutics. Nanofiber-based hydrogels are useful delivery systems in biomedical applications due to their drug loading capability and controlled release. Here, a biocompatible visible light-triggered in situ-gelling drug delivery system is demonstrated consisting of ascorbyl palmitate nanofibers and gelatin methacryloyl polymer.
基于纳米纤维的水凝胶给药系统最近在生物医学应用中显示出巨大的潜力，特别是由于其超细纳米纤维的高表面体积比和携带低溶解度药物的能力。在此，我们介绍一种由抗坏血酸棕榈酸酯（AP）纳米纤维和明胶甲基丙烯酰聚合物组成的可见光触发原位胶凝药物载体（GAP Gel）。抗坏血酸棕榈酸酯（AP）纳米纤维通过分子间相互作用与疏水性载药核心形成自组装结构。我们证明，AP 纳米纤维的亲水性外围使其能够通过氢键与其他亲水性分子相互作用。AP 纳米纤维的存在以浓度依赖的方式显著增强了 GAP 凝胶的粘弹性。此外，GAP 凝胶在负载疏水性抗生素时显示出体外生物相容性和持续给药效果。同样，当 GAP 凝胶以各种形式植入免疫功能正常的小鼠体内时，也显示出良好的体内生物相容性。最后，GAP 凝胶在三维环境中培养 7 天后仍能保持细胞活力，从而使其成为一种前景广阔的多功能水凝胶平台，用于输送生物治疗药物。基于纳米纤维的水凝胶具有药物负载能力和可控释放特性，是生物医学应用中非常有用的递送系统。本文展示了一种由抗坏血酸棕榈酸酯纳米纤维和明胶甲基丙烯酰聚合物组成的生物相容性可见光触发原位胶凝给药系统。
{"title":"Ascorbyl palmitate nanofiber-reinforced hydrogels for drug delivery in soft issues","authors":"Yasmeen Shamiya, Aishik Chakraborty, Alap Ali Zahid, Nicholas Bainbridge, Jingyuan Guan, Biao Feng, Dominic Pjontek, Subrata Chakrabarti, Arghya Paul","doi":"10.1038/s43246-024-00641-x","DOIUrl":"10.1038/s43246-024-00641-x","url":null,"abstract":"Nanofiber-based hydrogel delivery systems have recently shown great potential in biomedical applications, specifically due to their high surface-to-volume ratio of ultra-fine nanofibers and their ability to carry low solubility drugs. Herein, we introduce a visible light-triggered in situ-gelling drug vehicle (GAP Gel) composed of ascorbyl palmitate (AP) nanofibers and gelatin methacryloyl polymer. AP nanofibers form self-assembled structures through intermolecular interactions with a hydrophobic drug-loading core. We demonstrate that the hydrophilic periphery of AP nanofibers allows them to interact with other hydrophilic molecules via hydrogen bonds. The presence of AP nanofibers significantly enhances the viscoelasticity of GAP Gel in a concentration-dependent manner. Further, GAP Gel shows in vitro biocompatibility and sustained drug delivery efficacy when loaded with a hydrophobic antibiotic. Likewise, GAP Gel shows excellent in vivo biocompatibility when implanted in immunocompetent mice in various forms. Lastly, GAP Gels maintain cell viability when cultured in a 3D-environment over 7 days, establishing it as a promising and versatile hydrogel platform for the delivery of biotherapeutics. Nanofiber-based hydrogels are useful delivery systems in biomedical applications due to their drug loading capability and controlled release. Here, a biocompatible visible light-triggered in situ-gelling drug delivery system is demonstrated consisting of ascorbyl palmitate nanofibers and gelatin methacryloyl polymer.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00641-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142275109","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-20DOI: 10.1038/s43246-024-00637-7
Lucas Carolus van Laake, Johannes Tesse Bastiaan Overvelde
Soft robotic actuation concepts meet and sometimes exceed their natural counterparts. In contrast, artificially recreating natural levels of autonomy is still an unmet challenge. Here, we come to this conclusion after defining a measure of energy- and control-autonomy and classifying a representative selection of soft robots. We argue that, in order to advance the field, we should focus our attention on interactions between soft robots and their environment, because in nature autonomy is also achieved in interdependence. If we better understand how interactions with an environment are leveraged in nature, this will enable us to design bio-inspired soft robots with much greater autonomy in the future. Naturally occurring organisms continue to provide inspiration for advanced functionality in soft robots. This Perspective discusses how achieving autonomy in robots will require interactions with their environment to be taken into consideration in their design.
{"title":"Bio-inspired autonomy in soft robots","authors":"Lucas Carolus van Laake, Johannes Tesse Bastiaan Overvelde","doi":"10.1038/s43246-024-00637-7","DOIUrl":"10.1038/s43246-024-00637-7","url":null,"abstract":"Soft robotic actuation concepts meet and sometimes exceed their natural counterparts. In contrast, artificially recreating natural levels of autonomy is still an unmet challenge. Here, we come to this conclusion after defining a measure of energy- and control-autonomy and classifying a representative selection of soft robots. We argue that, in order to advance the field, we should focus our attention on interactions between soft robots and their environment, because in nature autonomy is also achieved in interdependence. If we better understand how interactions with an environment are leveraged in nature, this will enable us to design bio-inspired soft robots with much greater autonomy in the future. Naturally occurring organisms continue to provide inspiration for advanced functionality in soft robots. This Perspective discusses how achieving autonomy in robots will require interactions with their environment to be taken into consideration in their design.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00637-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142275108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-19DOI: 10.1038/s43246-024-00628-8
Lara G. Dresser, Casper Kunstmann-Olsen, Donato Conteduca, Christopher M. Hofmair, Nathan Smith, Laura Clark, Steven Johnson, J. Carlos Penedo, Mark C. Leake, Steven D. Quinn
Detergent-induced vesicle interactions, critical for applications including virus inactivation, varies according to the detergent type and membrane composition, but the underlying mechanistic details remain underexplored. Here, we use a lipid mixing assay based on Förster resonance energy transfer (FRET), and single-vesicle characterization approaches to identify that sub-micron-sized vesicles are induced to fuse by the non-ionic detergent Triton-X-100. We demonstrate that the process is a multi-step mechanism, characterized by discrete values of FRET efficiency between membrane-embedded fluorophores, and involves permeabilization, vesicle docking, hemi-fusion and full lipid mixing at sub-solubilizing detergent concentrations. We also dissect the kinetics of vesicle fusion to surface-tethered vesicles using a label-free quartz-crystal microbalance with dissipation monitoring approach, opening a platform for biotechnology applications. The presented strategies provide mechanistic insight into the dynamics of vesicle fusion and have implications for applications including drug delivery and sensor development where transport and manipulation of encapsulated cargo is essential. Detergent-induced membrane interactions are important for biotechnology applications but their mechanism is still not well understood. Here, sub-micron-sized vesicles are shown to fuse by a non-ionic detergent, involving permeabilization, vesicle docking, hemi-fusion, and full lipid mixing steps.
{"title":"Multiple intermediates in the detergent-induced fusion of lipid vesicles","authors":"Lara G. Dresser, Casper Kunstmann-Olsen, Donato Conteduca, Christopher M. Hofmair, Nathan Smith, Laura Clark, Steven Johnson, J. Carlos Penedo, Mark C. Leake, Steven D. Quinn","doi":"10.1038/s43246-024-00628-8","DOIUrl":"10.1038/s43246-024-00628-8","url":null,"abstract":"Detergent-induced vesicle interactions, critical for applications including virus inactivation, varies according to the detergent type and membrane composition, but the underlying mechanistic details remain underexplored. Here, we use a lipid mixing assay based on Förster resonance energy transfer (FRET), and single-vesicle characterization approaches to identify that sub-micron-sized vesicles are induced to fuse by the non-ionic detergent Triton-X-100. We demonstrate that the process is a multi-step mechanism, characterized by discrete values of FRET efficiency between membrane-embedded fluorophores, and involves permeabilization, vesicle docking, hemi-fusion and full lipid mixing at sub-solubilizing detergent concentrations. We also dissect the kinetics of vesicle fusion to surface-tethered vesicles using a label-free quartz-crystal microbalance with dissipation monitoring approach, opening a platform for biotechnology applications. The presented strategies provide mechanistic insight into the dynamics of vesicle fusion and have implications for applications including drug delivery and sensor development where transport and manipulation of encapsulated cargo is essential. Detergent-induced membrane interactions are important for biotechnology applications but their mechanism is still not well understood. Here, sub-micron-sized vesicles are shown to fuse by a non-ionic detergent, involving permeabilization, vesicle docking, hemi-fusion, and full lipid mixing steps.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00628-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-19DOI: 10.1038/s43246-024-00639-5
Swarbhanu Ghosh, Parisa A. Ariya
Anthropogenic climate change drastically affects our planet, with CO2 being the most critical gaseous driver. Despite the existing carbon dioxide capture and transformation, there is much need for innovative carbon dioxide hydrogenation catalysts with excellent selectivity. Here, we present a fast, effective, and sustainable route for coupling diverse alcohols, amines and amides with CO2 via heterogenization of a natural metal-based homogeneous catalyst through decorating on functionalized graphene oxide (GO). Combined synthetic, experimental, and theoretical studies unravel mechanistic routes to convergent 4‑electron reduction of CO2 under mild conditions. We successfully replace the toxic and expensive ruthenium species with inexpensive, ubiquitously available and recyclable iron. This iron-based functionalized graphene oxide (denoted as Fe@GO-EDA, where EDA represents ethylenediamine) functions as an efficient catalyst for the selective conversion of CO2 into a formaldehyde oxidation level, thus opening the door for interesting molecular structures using CO2 as a C1 source. Overall, this work describes an intriguing heterogeneous platform for the selective synthesis of valuable methylene-bridged compounds via 4‑electron reduction of CO2. Carbon dioxide in the atmosphere can be captured and transformed to useful chemicals with hydrogenation catalysts. Here, iron-functionalized graphene oxide-based catalyst functions as an effective catalyst for the selective conversion of carbon dioxide into a formaldehyde oxidation level.
人为气候变化严重影响着我们的地球，而二氧化碳是最关键的气体驱动因素。尽管已有二氧化碳捕获和转化技术，但我们仍亟需具有优异选择性的创新型二氧化碳氢化催化剂。在此，我们提出了一种快速、有效、可持续的路线，通过在功能化氧化石墨烯（GO）上装饰天然金属基均相催化剂，将多种醇、胺和酰胺与二氧化碳进行异质化偶联。结合合成、实验和理论研究，我们揭示了在温和条件下实现 CO2 4 电子还原的机理路线。我们成功地用廉价、普遍可用且可回收的铁取代了有毒且昂贵的钌。这种铁基功能化氧化石墨烯（标记为 Fe@GO-EDA，其中 EDA 代表乙二胺）可作为一种高效催化剂，将 CO2 选择性地转化为甲醛氧化级，从而为利用 CO2 作为 C1 源的有趣分子结构打开了大门。总之，这项工作描述了一个有趣的异质平台，可通过 CO2 的 4 电子还原选择性合成有价值的亚甲基桥化合物。
{"title":"Selective reductive conversion of CO2 to CH2-bridged compounds by using a Fe-functionalized graphene oxide-based catalyst","authors":"Swarbhanu Ghosh, Parisa A. Ariya","doi":"10.1038/s43246-024-00639-5","DOIUrl":"10.1038/s43246-024-00639-5","url":null,"abstract":"Anthropogenic climate change drastically affects our planet, with CO2 being the most critical gaseous driver. Despite the existing carbon dioxide capture and transformation, there is much need for innovative carbon dioxide hydrogenation catalysts with excellent selectivity. Here, we present a fast, effective, and sustainable route for coupling diverse alcohols, amines and amides with CO2 via heterogenization of a natural metal-based homogeneous catalyst through decorating on functionalized graphene oxide (GO). Combined synthetic, experimental, and theoretical studies unravel mechanistic routes to convergent 4‑electron reduction of CO2 under mild conditions. We successfully replace the toxic and expensive ruthenium species with inexpensive, ubiquitously available and recyclable iron. This iron-based functionalized graphene oxide (denoted as Fe@GO-EDA, where EDA represents ethylenediamine) functions as an efficient catalyst for the selective conversion of CO2 into a formaldehyde oxidation level, thus opening the door for interesting molecular structures using CO2 as a C1 source. Overall, this work describes an intriguing heterogeneous platform for the selective synthesis of valuable methylene-bridged compounds via 4‑electron reduction of CO2. Carbon dioxide in the atmosphere can be captured and transformed to useful chemicals with hydrogenation catalysts. Here, iron-functionalized graphene oxide-based catalyst functions as an effective catalyst for the selective conversion of carbon dioxide into a formaldehyde oxidation level.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00639-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255285","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00636-8
Chunyang Zhang, Nam-Gyu Park
Although perovskite solar cells (PSCs) are promising next generation photovoltaics, the production of PSCs might be hampered by complex and inefficient procedures. This Review outlines important advances in materials and methods for the cost-effective manufacturing of PSCs, including precursor synthesis, selection criteria for precursors based on chemistry, additive engineering, and deposition techniques. The goal of these technologies is not only to improve the performance and stability of PSCs, but also to significantly reduce their manufacturing costs. These advances are critical to the commercialization of PSCs, in terms of making them viable and cost-effective. The scalable and cost-effective synthesis of perovskite solar cells is dependent on materials chemistry and the synthesis technique. This Review discusses these considerations, including selecting a suitable perovskite pre-cursor, additive engineering, and the deposition process.
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Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00629-7
Zainah A. AlDhawi, Ridha Hamdi, Mahmoud A. Abdulhamid
Photocatalytic degradation of organic pollutants is an essential technology for various environmental applications. However, the effectiveness of most photocatalysts is restricted to light. Herein, we report metal-free catalysts derived from intrinsically microporous polyimide for persistence in photocatalytic degradation of dyes. We systematically investigate the effect of porosity and functionality on photocatalytic efficiency. Both the pristine 4,4′-(hexafluoroisopropylidene)diphthalic anhydride-3,3′-dimethylnaphthidine and its thermally annealed counterpart at 530 °C exhibit high charge storage capabilities, enabling continuous photodegradation in the absence of light. The pre-irradiated catalyst exhibits an approximately 99% degradation of the dye, with a ~40% improvement relative to the non-pre-irradiated sample. We studied the influence of the chemical structure and porosity on the photocatalytic degradation efficiency in darkness by varying the polyimide chemical structure using different diamines. This research underscores the potential of polymers with intrinsic microporosity for application in the continuous degradation of dyes, contributing to the pursuit of cleaner water. Photodegradation of pollutants is important to produce clean water but their activities are restricted during nighttime. Here, metal-free catalysts derived from intrinsically microporous polyimide show efficient photocatalytic degradation activities of dyes under light and darkness.
光催化降解有机污染物是各种环境应用中的一项重要技术。然而，大多数光催化剂的功效仅限于光。在此，我们报告了由固有微孔聚酰亚胺衍生的无金属催化剂在光催化降解染料中的持久性。我们系统地研究了多孔性和功能性对光催化效率的影响。原始的 4,4′-(六氟异亚丙基)二邻苯二甲酸酐-3,3′-二甲基萘啶及其在 530 °C 下热退火的对应物都表现出很高的电荷储存能力，能在无光条件下持续光降解。预辐照催化剂的染料降解率约为 99%，与未经预辐照的样品相比提高了约 40%。我们通过使用不同的二胺改变聚酰亚胺的化学结构，研究了化学结构和孔隙率对黑暗中光催化降解效率的影响。这项研究强调了具有固有微孔的聚合物在持续降解染料方面的应用潜力，有助于实现更清洁的水质。
{"title":"Intrinsically microporous polyimide-based metal-free catalysts for round-the-clock photodegradation of organic pollutants","authors":"Zainah A. AlDhawi, Ridha Hamdi, Mahmoud A. Abdulhamid","doi":"10.1038/s43246-024-00629-7","DOIUrl":"10.1038/s43246-024-00629-7","url":null,"abstract":"Photocatalytic degradation of organic pollutants is an essential technology for various environmental applications. However, the effectiveness of most photocatalysts is restricted to light. Herein, we report metal-free catalysts derived from intrinsically microporous polyimide for persistence in photocatalytic degradation of dyes. We systematically investigate the effect of porosity and functionality on photocatalytic efficiency. Both the pristine 4,4′-(hexafluoroisopropylidene)diphthalic anhydride-3,3′-dimethylnaphthidine and its thermally annealed counterpart at 530 °C exhibit high charge storage capabilities, enabling continuous photodegradation in the absence of light. The pre-irradiated catalyst exhibits an approximately 99% degradation of the dye, with a ~40% improvement relative to the non-pre-irradiated sample. We studied the influence of the chemical structure and porosity on the photocatalytic degradation efficiency in darkness by varying the polyimide chemical structure using different diamines. This research underscores the potential of polymers with intrinsic microporosity for application in the continuous degradation of dyes, contributing to the pursuit of cleaner water. Photodegradation of pollutants is important to produce clean water but their activities are restricted during nighttime. Here, metal-free catalysts derived from intrinsically microporous polyimide show efficient photocatalytic degradation activities of dyes under light and darkness.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00629-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255335","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-18DOI: 10.1038/s43246-024-00634-w
Seong-Hoon Jang, Yukitoshi Motome
The Kitaev honeycomb model plays a pivotal role in the quest for quantum spin liquids, in which fractional quasiparticles would provide applications in decoherence-free topological quantum computing. The key ingredient is the bond-dependent Ising-type interactions, dubbed the Kitaev interactions, which require strong entanglement between spin and orbital degrees of freedom. Here we investigate the identification and design of rare-earth materials displaying robust Kitaev interactions. We scrutinize all possible 4f electron configurations, which require up to 6+ million intermediate states in the perturbation processes, by developing a parallel computational program designed for massive-scale calculations. Our analysis reveals a predominant interplay between the isotropic Heisenberg J and anisotropic Kitaev K interactions across all realizations of the Kramers doublets. Remarkably, instances featuring 4f3 and 4f11 configurations showcase the prevalence of K over J, presenting unexpected prospects for exploring the Kitaev quantum spin liquids in compounds, including Nd3+ and Er3+, respectively. Kitaev magnets are interesting as they can host quantum spin liquid phases and fractional quasiparticles for decoherence-free topological quantum computing. Here, a parallel computational program explores all possible 4f electron configurations of rare-earth Kitaev materials, identifying those configurations, such as 4f3 and 4f11 in Nd3+ and Er3+ compounds, where anisotropic Kitaev interactions prevail over isotropic Heisenberg exchange.
{"title":"Exploring rare-earth Kitaev magnets by massive-scale computational analysis","authors":"Seong-Hoon Jang, Yukitoshi Motome","doi":"10.1038/s43246-024-00634-w","DOIUrl":"10.1038/s43246-024-00634-w","url":null,"abstract":"The Kitaev honeycomb model plays a pivotal role in the quest for quantum spin liquids, in which fractional quasiparticles would provide applications in decoherence-free topological quantum computing. The key ingredient is the bond-dependent Ising-type interactions, dubbed the Kitaev interactions, which require strong entanglement between spin and orbital degrees of freedom. Here we investigate the identification and design of rare-earth materials displaying robust Kitaev interactions. We scrutinize all possible 4f electron configurations, which require up to 6+ million intermediate states in the perturbation processes, by developing a parallel computational program designed for massive-scale calculations. Our analysis reveals a predominant interplay between the isotropic Heisenberg J and anisotropic Kitaev K interactions across all realizations of the Kramers doublets. Remarkably, instances featuring 4f3 and 4f11 configurations showcase the prevalence of K over J, presenting unexpected prospects for exploring the Kitaev quantum spin liquids in compounds, including Nd3+ and Er3+, respectively. Kitaev magnets are interesting as they can host quantum spin liquid phases and fractional quasiparticles for decoherence-free topological quantum computing. Here, a parallel computational program explores all possible 4f electron configurations of rare-earth Kitaev materials, identifying those configurations, such as 4f3 and 4f11 in Nd3+ and Er3+ compounds, where anisotropic Kitaev interactions prevail over isotropic Heisenberg exchange.","PeriodicalId":10589,"journal":{"name":"Communications Materials","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s43246-024-00634-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142255248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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