Xiaoyang Yu, Huan Li, Ke Qiu, Ning Kang, Zhoumei Xu, Qian Li, Shouxiang Lu
Liquid foams with tunable and photoresponsive stabilities and mechanical properties are highly desired in many domains, including the chemical and environmental protection industries. Here, we constructed photoresponsive liquid foams by structuring the interfacial adsorption layers and nanoparticle‐embedded Plateau borders of the foam with biodegradable components. These foams exhibited ultrahigh foam stability but were easily destroyed by light, leading to a clean recovery of the liquid phase. In the absence of light, the hydroxypropyl cellulose (HPC) coils in the foam formed mechanically strong liquid films or “cohesive states.” Under irradiation, the ultrathin black phosphorus nanosheets induced changes in the packing parameters of the HPC assemblies within the Plateau borders and led to coil‐to‐globule transitions of the HPC and formed unstable liquid films with a “mobile state.” The two interfacial states were reversibly and repeatedly switched by turning the light on and off, which caused rapid bubble coalescence and foam collapse, and we also proved that this destabilizing mechanism was inhibited by cellulose nanocrystals. This work provides an environmentally friendly approach to controlling foam stability, and the proposed strategy can be expanded to the production of multiresponsive fully liquid objects in theory.
{"title":"Light‐driven reversible and repeatable switching between ultrastable and unstable liquid foam","authors":"Xiaoyang Yu, Huan Li, Ke Qiu, Ning Kang, Zhoumei Xu, Qian Li, Shouxiang Lu","doi":"10.1002/smm2.1275","DOIUrl":"https://doi.org/10.1002/smm2.1275","url":null,"abstract":"Liquid foams with tunable and photoresponsive stabilities and mechanical properties are highly desired in many domains, including the chemical and environmental protection industries. Here, we constructed photoresponsive liquid foams by structuring the interfacial adsorption layers and nanoparticle‐embedded Plateau borders of the foam with biodegradable components. These foams exhibited ultrahigh foam stability but were easily destroyed by light, leading to a clean recovery of the liquid phase. In the absence of light, the hydroxypropyl cellulose (HPC) coils in the foam formed mechanically strong liquid films or “cohesive states.” Under irradiation, the ultrathin black phosphorus nanosheets induced changes in the packing parameters of the HPC assemblies within the Plateau borders and led to coil‐to‐globule transitions of the HPC and formed unstable liquid films with a “mobile state.” The two interfacial states were reversibly and repeatedly switched by turning the light on and off, which caused rapid bubble coalescence and foam collapse, and we also proved that this destabilizing mechanism was inhibited by cellulose nanocrystals. This work provides an environmentally friendly approach to controlling foam stability, and the proposed strategy can be expanded to the production of multiresponsive fully liquid objects in theory.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139616190","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Recently, the collective behavior of micro/nanorobots has shown unprecedented potential in biomedicine and environmental remediation. Collective behavior can work more efficiently, adaptively, and robustly than individual micro/nanorobots. The paradigm of collective behavior needs to be understood in different dimensions, including from individual to cluster, from planar to spatial, and from mono‐functional to multifunctional. In this review, the focus will be on summarizing the achievements of collective control of micro/nanorobot swarms in recent years from different dimensions, in an attempt to better understand how the structure and materials of individuals should be designed, how collective behavior should be implemented, and how robots are functionalized to cope with practical applications under the introduction of collective control. The opportunities and challenges that collective control faces at this stage are illustrated to provide perspectives for its future development.
{"title":"Multi‐dimensional micro/nanorobots with collective behaviors","authors":"Bin Wang, Yuanyuan Lu","doi":"10.1002/smm2.1263","DOIUrl":"https://doi.org/10.1002/smm2.1263","url":null,"abstract":"Recently, the collective behavior of micro/nanorobots has shown unprecedented potential in biomedicine and environmental remediation. Collective behavior can work more efficiently, adaptively, and robustly than individual micro/nanorobots. The paradigm of collective behavior needs to be understood in different dimensions, including from individual to cluster, from planar to spatial, and from mono‐functional to multifunctional. In this review, the focus will be on summarizing the achievements of collective control of micro/nanorobot swarms in recent years from different dimensions, in an attempt to better understand how the structure and materials of individuals should be designed, how collective behavior should be implemented, and how robots are functionalized to cope with practical applications under the introduction of collective control. The opportunities and challenges that collective control faces at this stage are illustrated to provide perspectives for its future development.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139619874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Large‐sized and atomically thin two‐dimensional metal thiophosphate materials have been widely exploited in detectors due to their rich physical/chemical properties of high surface area and massive adjustable sites. However, existing production methods are limited in terms of meeting the demanding challenges in achieving the scalable fabrication of high‐quality nanomaterials under mild conditions. Here, we develop a facile intercalation–exfoliation method that can fabricate large lateral size (>23 μm) and few‐layer LiInP2S6 nanosheets with high crystalline quality fast. Due to the advantage of hydrophilicity of lithium, swelled interlayer spacing can be obtained, which enables the rapid exfoliation by only slight manual shaking within tens of seconds. Concomitantly, the inorganic LiInP2S6 film manufactured by nanosheets has inter‐connected ionic channels, which can be adjusted on the basis of the water content, enabling tunable ionic conductivity. As a result, ionic conductor films using ions as charge carriers can achieve high water response with good repeatability and excellent long‐term stability in a wide moisture range. Moreover, the as‐prepared detector has excellent capability in real‐time noncontact human–machine interfacing. This study, not only is a powerful strategy for the fabrication of large‐sized and high‐quality nanosheets presented but also proof for the promising development of iontronic devices in new applications.
{"title":"Manual shaking exfoliation of large‐size two‐dimensional LiInP2S6 nanosheets with exponential change in ionic conductivity for water detection","authors":"Jianing Liang, Zongdong Sun, Chaoqi Zhu, Shuhao Wang, Cheng Zeng, Dawen Zeng, Tianyou Zhai, Huiqiao Li","doi":"10.1002/smm2.1266","DOIUrl":"https://doi.org/10.1002/smm2.1266","url":null,"abstract":"Large‐sized and atomically thin two‐dimensional metal thiophosphate materials have been widely exploited in detectors due to their rich physical/chemical properties of high surface area and massive adjustable sites. However, existing production methods are limited in terms of meeting the demanding challenges in achieving the scalable fabrication of high‐quality nanomaterials under mild conditions. Here, we develop a facile intercalation–exfoliation method that can fabricate large lateral size (>23 μm) and few‐layer LiInP2S6 nanosheets with high crystalline quality fast. Due to the advantage of hydrophilicity of lithium, swelled interlayer spacing can be obtained, which enables the rapid exfoliation by only slight manual shaking within tens of seconds. Concomitantly, the inorganic LiInP2S6 film manufactured by nanosheets has inter‐connected ionic channels, which can be adjusted on the basis of the water content, enabling tunable ionic conductivity. As a result, ionic conductor films using ions as charge carriers can achieve high water response with good repeatability and excellent long‐term stability in a wide moisture range. Moreover, the as‐prepared detector has excellent capability in real‐time noncontact human–machine interfacing. This study, not only is a powerful strategy for the fabrication of large‐sized and high‐quality nanosheets presented but also proof for the promising development of iontronic devices in new applications.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139618393","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Microbial fuel cells (MFCs) benefit from the introduction of iron in the anode, as its multiple valence states and high electron‐catalytic activity led to improved power densities in MFCs. However, the effect of long‐term Fe3+ release into the electrolyte on the power density of MFCs is often overlooked. Herein, an anode consisting of a three‐dimensional iron foam uniformly coated by reduced graphene oxide (rGO/IF) with a suitable loading density (8 g/m2) and a large specific surface area (0.05 m2/g) for high‐density bacterial loading was prepared. The hybrid cells based on the rGO/IF anode exhibit a maximum power density of 5330 ± 76 mW/m2 contributed by MFCs and galvanic cells. The rGO/IF anode enables continuous Fe3+ release for high electron‐catalytic activity in the electrolyte during the discharging of the galvanic cells. As a result, the hybrid cells showed a power density of 2107 ± 64 mW/m2 after four cycles, facilitated through reversible conversion between Fe3+ and Fe2+ in the electrolyte to accelerate electron transfer efficiency. The results indicate that the rGO/IF anode can be used for designing and fabricating high‐power MFCs by optimizing the rate of release of Fe3+ in the electrolyte.
{"title":"High‐power microbial‐fuel‐based hybrid cells with three‐dimensional graphene‐coated iron foam as an anode control Fe3+ release","authors":"Zijie Wu, Zhengyang Ni, Mengmeng Qin, Baocai Zhang, Qijing Liu, Fulai Zhao, Gejun Liu, Peng Long, Feng Li, Huitao Yu, Hao Song, Yiyu Feng, Wei Feng","doi":"10.1002/smm2.1267","DOIUrl":"https://doi.org/10.1002/smm2.1267","url":null,"abstract":"Microbial fuel cells (MFCs) benefit from the introduction of iron in the anode, as its multiple valence states and high electron‐catalytic activity led to improved power densities in MFCs. However, the effect of long‐term Fe3+ release into the electrolyte on the power density of MFCs is often overlooked. Herein, an anode consisting of a three‐dimensional iron foam uniformly coated by reduced graphene oxide (rGO/IF) with a suitable loading density (8 g/m2) and a large specific surface area (0.05 m2/g) for high‐density bacterial loading was prepared. The hybrid cells based on the rGO/IF anode exhibit a maximum power density of 5330 ± 76 mW/m2 contributed by MFCs and galvanic cells. The rGO/IF anode enables continuous Fe3+ release for high electron‐catalytic activity in the electrolyte during the discharging of the galvanic cells. As a result, the hybrid cells showed a power density of 2107 ± 64 mW/m2 after four cycles, facilitated through reversible conversion between Fe3+ and Fe2+ in the electrolyte to accelerate electron transfer efficiency. The results indicate that the rGO/IF anode can be used for designing and fabricating high‐power MFCs by optimizing the rate of release of Fe3+ in the electrolyte.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139618140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuqiong Sun, J. Huang, Yan Cheng, Jing Zhang, Yi Shi, Lijia Pan
Gesture recognition utilizing flexible strain sensors is a highly valuable technology widely applied in human–machine interfaces. However, achieving rapid detection of subtle motions and timely processing of dynamic signals remain a challenge for sensors. Here, highly resilient and durable ionogels are developed by introducing micro‐scale incompatible phases in macroscopic homogeneous polymeric network. The compatible network disperses in conductive ionic liquid to form highly resilient and stretchable skeleton, while incompatible phase forms hydrogen bonds to dissipate energy thus strengthening the ionogels. The ionogels‐derived strain sensors show highly sensitivity, fast response time (<10 ms), low detection limit (~50 μm), and remarkable durability (>5000 cycles), allowing for precise monitoring of human motions. More importantly, a self‐adaptive recognition program empowered by deep‐learning algorithms is designed to compensate for sensors, creating a comprehensive system capable of dynamic gesture recognition. This system can comprehensively analyze both the temporal and spatial features of sensor data, enabling deeper understanding of the dynamic process underlying gestures. The system accurately classifies 10 hand gestures across five participants with impressive accuracy of 93.66%. Moreover, it maintains robust recognition performance without the need for further training even when different sensors or subjects are involved. This technological breakthrough paves the way for intuitive and seamless interaction between humans and machines, presenting significant opportunities in diverse applications, such as human–robot interaction, virtual reality control, and assistive devices for the disabled individuals.
{"title":"High‐accuracy dynamic gesture recognition: A universal and self‐adaptive deep‐learning‐assisted system leveraging high‐performance ionogels‐based strain sensors","authors":"Yuqiong Sun, J. Huang, Yan Cheng, Jing Zhang, Yi Shi, Lijia Pan","doi":"10.1002/smm2.1269","DOIUrl":"https://doi.org/10.1002/smm2.1269","url":null,"abstract":"Gesture recognition utilizing flexible strain sensors is a highly valuable technology widely applied in human–machine interfaces. However, achieving rapid detection of subtle motions and timely processing of dynamic signals remain a challenge for sensors. Here, highly resilient and durable ionogels are developed by introducing micro‐scale incompatible phases in macroscopic homogeneous polymeric network. The compatible network disperses in conductive ionic liquid to form highly resilient and stretchable skeleton, while incompatible phase forms hydrogen bonds to dissipate energy thus strengthening the ionogels. The ionogels‐derived strain sensors show highly sensitivity, fast response time (<10 ms), low detection limit (~50 μm), and remarkable durability (>5000 cycles), allowing for precise monitoring of human motions. More importantly, a self‐adaptive recognition program empowered by deep‐learning algorithms is designed to compensate for sensors, creating a comprehensive system capable of dynamic gesture recognition. This system can comprehensively analyze both the temporal and spatial features of sensor data, enabling deeper understanding of the dynamic process underlying gestures. The system accurately classifies 10 hand gestures across five participants with impressive accuracy of 93.66%. Moreover, it maintains robust recognition performance without the need for further training even when different sensors or subjects are involved. This technological breakthrough paves the way for intuitive and seamless interaction between humans and machines, presenting significant opportunities in diverse applications, such as human–robot interaction, virtual reality control, and assistive devices for the disabled individuals.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139529186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Artificial skin with tactile perceptions is anticipated to play a pivotal role in next‐generation robotic and medical devices. The primary challenge lies in creating a biomimetic system that seamlessly integrates with the human body and biological systems. The authors have developed an electronic skin (e‐skin) that imitates the biological sensorimotor loop through medium‐scale circuit integration, boasting low power consumption and solid‐state synaptic transistors.
{"title":"A low‐voltage‐driven, neuromorphic sensorimotor loop for monolithic soft prosthetic e‐skin","authors":"Xiangxiang Li, Darakhshan Mehvish, Hui Yang","doi":"10.1002/smm2.1248","DOIUrl":"https://doi.org/10.1002/smm2.1248","url":null,"abstract":"Artificial skin with tactile perceptions is anticipated to play a pivotal role in next‐generation robotic and medical devices. The primary challenge lies in creating a biomimetic system that seamlessly integrates with the human body and biological systems. The authors have developed an electronic skin (e‐skin) that imitates the biological sensorimotor loop through medium‐scale circuit integration, boasting low power consumption and solid‐state synaptic transistors.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139627057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yifan Xie, Chenming Ding, Qingqing Jin, Lei Zheng, Yunqi Xu, Hongmei Xiao, Miao Cheng, Yanqin Zhang, Guanhua Yang, Mengmeng Li, Ling Li, Ming Liu
With the rapid development of advanced technologies in the Internet of Things era, higher requirements are needed for next‐generation electronic devices. Fortunately, organic thin film transistors (OTFTs) provide an effective solution for electronic skin and flexible wearable devices due to their intrinsic features of mechanical flexibility, lightweight, simple fabrication process, and good biocompatibility. So far considerable efforts have been devoted to this research field. This article reviews recent advances in various promising and state‐of‐the‐art OTFTs as well as related integrated circuits with the main focuses on: (I) material categories of high‐mobility organic semiconductors for both individual transistors and integrated circuits; (II) effective device architectures and processing techniques for large‐area fabrication; (III) important performance metrics of organic integrated circuits and realization of digital and analog devices for future smart life; (IV) applicable analytical models and design flow to accelerate the circuit design. In addition, the emerging challenges of OTFT‐based integrated circuits, such as transistor uniformity and stability are also discussed, and the possible methods to solve these problems at both transistor and circuit levels are summarized.
{"title":"Organic transistor‐based integrated circuits for future smart life","authors":"Yifan Xie, Chenming Ding, Qingqing Jin, Lei Zheng, Yunqi Xu, Hongmei Xiao, Miao Cheng, Yanqin Zhang, Guanhua Yang, Mengmeng Li, Ling Li, Ming Liu","doi":"10.1002/smm2.1261","DOIUrl":"https://doi.org/10.1002/smm2.1261","url":null,"abstract":"With the rapid development of advanced technologies in the Internet of Things era, higher requirements are needed for next‐generation electronic devices. Fortunately, organic thin film transistors (OTFTs) provide an effective solution for electronic skin and flexible wearable devices due to their intrinsic features of mechanical flexibility, lightweight, simple fabrication process, and good biocompatibility. So far considerable efforts have been devoted to this research field. This article reviews recent advances in various promising and state‐of‐the‐art OTFTs as well as related integrated circuits with the main focuses on: (I) material categories of high‐mobility organic semiconductors for both individual transistors and integrated circuits; (II) effective device architectures and processing techniques for large‐area fabrication; (III) important performance metrics of organic integrated circuits and realization of digital and analog devices for future smart life; (IV) applicable analytical models and design flow to accelerate the circuit design. In addition, the emerging challenges of OTFT‐based integrated circuits, such as transistor uniformity and stability are also discussed, and the possible methods to solve these problems at both transistor and circuit levels are summarized.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139452672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xin Kong, Bin Liu, Zhongqiu Tong, Rui Bao, Jianhong Yi, Shuyu Bu, Yunpeng Liu, Pengfei Wang, Chun‐Sing Lee, Wenjun Zhang
Metallic phthalocyanines are promising electrocatalysts for CO2 reduction reaction (CO2RR). However, their catalytic activity and stability (especially under high potential) are still unsatisfactory. Herein, we synthesized a covalent organic polymer (COP‐CoPc) by introducing charge‐switchable viologen ligands into cobalt phthalocyanine (CoPc). The COP‐CoPc exhibits great activity for CO2RR, including a high Faradaic efficiency over a wide potential window and the highest CO partial current density among all ligand‐tuned phthalocyanine catalysts reported in the H‐type cell. Particularly, COP‐CoPc also shows great potential for practical applications, for example, a FECO of >95% is realized at a large current density of 150 mA/cm2 in a two‐electrode membrane electrode assembly reactor. Ex situ and in situ X‐ray absorption fine structure spectroscopy measurements and theory calculations reveal that when the charge‐switchable viologen ligands switch to neutral‐state ones, they can act as electron donors to enrich the electron density of Co centers in COP‐CoPc and enhance the desorption of *CO, thus improving the CO selectivity. Moreover, the excellent reversible redox capability of viologen ligands and the increased Co–N bonding strength in the Co–N4 sites enable COP‐CoPc to possess outstanding stability under elevated potentials and currents, enriching the knowledge of charge‐switchable ligands tailored CO2RR performance.
金属酞菁是一种很有前景的二氧化碳还原反应（CO2RR）电催化剂。然而，它们的催化活性和稳定性（尤其是在高电位下）仍不尽如人意。在此，我们通过在酞菁钴（CoPc）中引入电荷可切换的紫胶配体，合成了一种共价有机聚合物（COP-CoPc）。COP-CoPc 在 CO2RR 方面表现出极高的活性，包括在较宽的电位窗口内具有较高的法拉第效率，以及在 H 型电池中，在所有配体调谐酞菁催化剂中具有最高的 CO 部分电流密度。特别是，COP-CoPc 还显示出巨大的实际应用潜力，例如，在双电极膜电极组装反应器中，150 mA/cm2 的大电流密度下实现了 >95% 的 FECO。原位和原位 X 射线吸收精细结构光谱测量和理论计算表明，当电荷转换型紫胶配体转换为中性态配体时，它们可以充当电子供体，丰富 COP-CoPc 中 Co 中心的电子密度，增强 *CO 的解吸能力，从而提高 CO 的选择性。此外，紫胶配体优异的可逆氧化还原能力和 Co-N4 位点中 Co-N 键强度的增加，使 COP-CoPc 在高电位和高电流条件下具有出色的稳定性，丰富了电荷转换配体定制 CO2RR 性能的知识。
{"title":"Charge‐switchable ligand ameliorated cobalt polyphthalocyanine polymers for high‐current‐density electrocatalytic CO2 reduction","authors":"Xin Kong, Bin Liu, Zhongqiu Tong, Rui Bao, Jianhong Yi, Shuyu Bu, Yunpeng Liu, Pengfei Wang, Chun‐Sing Lee, Wenjun Zhang","doi":"10.1002/smm2.1262","DOIUrl":"https://doi.org/10.1002/smm2.1262","url":null,"abstract":"Metallic phthalocyanines are promising electrocatalysts for CO2 reduction reaction (CO2RR). However, their catalytic activity and stability (especially under high potential) are still unsatisfactory. Herein, we synthesized a covalent organic polymer (COP‐CoPc) by introducing charge‐switchable viologen ligands into cobalt phthalocyanine (CoPc). The COP‐CoPc exhibits great activity for CO2RR, including a high Faradaic efficiency over a wide potential window and the highest CO partial current density among all ligand‐tuned phthalocyanine catalysts reported in the H‐type cell. Particularly, COP‐CoPc also shows great potential for practical applications, for example, a FECO of >95% is realized at a large current density of 150 mA/cm2 in a two‐electrode membrane electrode assembly reactor. Ex situ and in situ X‐ray absorption fine structure spectroscopy measurements and theory calculations reveal that when the charge‐switchable viologen ligands switch to neutral‐state ones, they can act as electron donors to enrich the electron density of Co centers in COP‐CoPc and enhance the desorption of *CO, thus improving the CO selectivity. Moreover, the excellent reversible redox capability of viologen ligands and the increased Co–N bonding strength in the Co–N4 sites enable COP‐CoPc to possess outstanding stability under elevated potentials and currents, enriching the knowledge of charge‐switchable ligands tailored CO2RR performance.","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139452547","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xuan Gao, Kejiang Liu, Chang Su, Wei Zhang, Yuhang Dai, Ivan P Parkin, C. Carmalt, Guanjie He
{"title":"Outside Back Cover: Volume 5 Issue 1","authors":"Xuan Gao, Kejiang Liu, Chang Su, Wei Zhang, Yuhang Dai, Ivan P Parkin, C. Carmalt, Guanjie He","doi":"10.1002/smm2.1260","DOIUrl":"https://doi.org/10.1002/smm2.1260","url":null,"abstract":"","PeriodicalId":21794,"journal":{"name":"SmartMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139156927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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