Integrating hydrogen evolution reaction (HER) with hydrazine oxidation reaction (HzOR) has an encouraging prospect for the energy‐saving hydrogen production, demanding the high‐performance bifunctional HER/HzOR electrocatalyst. Ruthenium phosphide/doped carbon composites have exhibited superior activity toward multiple electrocatalytic reactions. To explore the decent water‐soluble precursors containing both N and P elements is highly attractive to facilely prepare metal phosphide/doped carbon composites. Herein, as one kind ecofriendly biomolecules, adenine nucleotide was first employed to selectively fabricate the highly pure RuP nanoparticles embedded into porous N,P‐codoped carbons (RuP/PNPC) with a straightforward “mix‐and‐pyrolyze” approach. The newly prepared RuP/PNPC only requires 4.0 and −83.0 mV at 10 mA/cm2 separately in alkaline HER and HzOR, outperforming most of reported electrocatalysts, together with the outstanding neutral bifunctional performance. Furthermore, the two‐electrode alkaline and neutral overall hydrazine splitting both exhibit significant power‐efficiency superiority to the corresponding overall water splitting with the voltage difference of larger than 2 V, which can be also easily driven by the fuel cells and solar cells with considerable H2 generation. Our report innovates the N‐ and P‐bearing adenine nucleotide to effortlessly synthesize the high‐quality RuP/doped carbon composite catalysts, highly potential as a universal platform for metal phosphide‐related functional materials.
将氢进化反应（HER）与肼氧化反应（HzOR）相结合，在节能制氢方面具有令人鼓舞的前景，这就需要高性能的 HER/HzOR 双功能电催化剂。磷化钌/掺杂碳复合材料在多种电催化反应中表现出卓越的活性。探索同时含有 N 和 P 元素的合适的水溶性前驱体对于轻松制备金属磷化物/掺杂碳复合材料极具吸引力。在本文中，腺嘌呤核苷酸作为一种生态友好型生物大分子，首先被用来选择性地制备高纯度的 RuP 纳米粒子，并将其嵌入多孔的 N、P-掺杂碳（RuP/PNPC）中。新制备的 RuP/PNPC 在 10 mA/cm2 的条件下，在碱性 HER 和 HzOR 中分别只需要 4.0 和 -83.0 mV 的电压，优于大多数已报道的电催化剂，同时具有出色的中性双功能性能。此外，在电压差大于 2 V 的情况下，双电极碱性和中性整体肼裂解的功率效率均明显优于相应的整体水裂解，这也很容易驱动燃料电池和太阳能电池产生大量的 H2。我们的报告创新性地利用含 N 和 P 的腺嘌呤核苷酸轻松合成了高质量的 RuP/掺杂碳复合催化剂，极有可能成为金属磷化相关功能材料的通用平台。
{"title":"Selectively nucleotide‐derived RuP on N,P‐codoped carbon with engineered mesopores for energy‐efficient hydrogen production assisted by hydrazine oxidation","authors":"Xiya Guan, Yu Sun, Simeng Zhao, Haibo Li, Suyuan Zeng, Qingxia Yao, Rui Li, Hongyan Chen, Konggang Qu","doi":"10.1002/sus2.186","DOIUrl":"https://doi.org/10.1002/sus2.186","url":null,"abstract":"Integrating hydrogen evolution reaction (HER) with hydrazine oxidation reaction (HzOR) has an encouraging prospect for the energy‐saving hydrogen production, demanding the high‐performance bifunctional HER/HzOR electrocatalyst. Ruthenium phosphide/doped carbon composites have exhibited superior activity toward multiple electrocatalytic reactions. To explore the decent water‐soluble precursors containing both N and P elements is highly attractive to facilely prepare metal phosphide/doped carbon composites. Herein, as one kind ecofriendly biomolecules, adenine nucleotide was first employed to selectively fabricate the highly pure RuP nanoparticles embedded into porous N,P‐codoped carbons (RuP/PNPC) with a straightforward “mix‐and‐pyrolyze” approach. The newly prepared RuP/PNPC only requires 4.0 and −83.0 mV at 10 mA/cm2 separately in alkaline HER and HzOR, outperforming most of reported electrocatalysts, together with the outstanding neutral bifunctional performance. Furthermore, the two‐electrode alkaline and neutral overall hydrazine splitting both exhibit significant power‐efficiency superiority to the corresponding overall water splitting with the voltage difference of larger than 2 V, which can be also easily driven by the fuel cells and solar cells with considerable H2 generation. Our report innovates the N‐ and P‐bearing adenine nucleotide to effortlessly synthesize the high‐quality RuP/doped carbon composite catalysts, highly potential as a universal platform for metal phosphide‐related functional materials.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140469258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jung Woo Hong, Harpalsinh H Rana, J. Park, Jun Su Kim, Sang Joon Lee, Gun-Woong Jang, Tae Hoon Kang, K. Shin, S. Baek, Wooseok Yang, Kwang Ho Kim, Ju‐Hyuk Lee, Ho Seok Park
The polymeric gel electrolytes are attractive owing to their higher ionic conductivities than those of dry polymer electrolytes and lowered water activity for enlarged potential window. However, the ionic conductivity and mechanical strength of the Na‐ion conducting polymeric gel electrolytes are limited by below 20 mS cm−1 and 2.2 MPa. Herein, we demonstrate Na‐ion conducting and flexible polymeric hydrogel electrolytes of the chemically coupled poly(diallyldimethylammonium chloride)‐dextrin‐N,N′‐methylene‐bis‐acrylamide film immersed in NaClO4 solution (ex‐DDA‐Dex + NaClO4) for flexible sodium‐ion hybrid capacitors (f‐NIHC). In particular, the anion exchange reaction and synergistic interaction of ex‐DDA‐Dex with the optimum ClO4− enable to greatly improve the ionic conductivity up to 27.63 mS cm−1 at 25°C and electrochemical stability window up to 2.6 V, whereas the double networking structure leads to achieve both the mechanical strength (7.48 MPa) and softness of hydrogel electrolytes. Therefore, the f‐NIHCs with the ex‐DDA‐Dex + NaClO4 achieved high specific and high‐rate capacities of 192.04 F g−1 at 500 mA g−1 and 116.06 F g−1 at 10 000 mA g−1, respectively, delivering a large energy density of 120.03 W h kg−1 at 906 W kg−1 and long cyclability of 70% over 500 cycles as well as demonstrating functional operation under mechanical stresses.
聚合凝胶电解质的吸引力在于其离子电导率高于干聚合物电解质，而且在扩大电位窗口时水活性较低。然而，Na 离子导电聚合物凝胶电解质的离子电导率和机械强度受到限制，分别低于 20 mS cm-1 和 2.2 MPa。在此，我们展示了用于柔性钠离子混合电容器（f-NIHC）的化学耦合聚（二烯丙基二甲基氯化铵）-糊精-N,N′-亚甲基双丙烯酰胺薄膜（ex-DDA-Dex + NaClO4）的Na离子导电柔性聚合物水凝胶电解质。其中，ex-DDA-Dex 与最佳 ClO4- 的阴离子交换反应和协同作用使其在 25°C 时的离子电导率高达 27.63 mS cm-1，电化学稳定性窗口高达 2.6 V，而双网络结构则使其同时具有水凝胶电解质的机械强度（7.48 MPa）和柔软性。因此，含有 ex-DDA-Dex + NaClO4 的 f-NIHC 在 500 mA g-1 和 10 000 mA g-1 下分别实现了 192.04 F g-1 和 116.06 F g-1 的高比容量和高倍率容量，在 906 W kg-1 下实现了 120.03 W h kg-1 的高能量密度，在 500 次循环中实现了 70% 的长循环性，并在机械应力下实现了功能性运行。
{"title":"High Na‐ion conductivity and mechanical integrity of anion‐exchanged polymeric hydrogel electrolytes for flexible sodium ion hybrid energy storage","authors":"Jung Woo Hong, Harpalsinh H Rana, J. Park, Jun Su Kim, Sang Joon Lee, Gun-Woong Jang, Tae Hoon Kang, K. Shin, S. Baek, Wooseok Yang, Kwang Ho Kim, Ju‐Hyuk Lee, Ho Seok Park","doi":"10.1002/sus2.182","DOIUrl":"https://doi.org/10.1002/sus2.182","url":null,"abstract":"The polymeric gel electrolytes are attractive owing to their higher ionic conductivities than those of dry polymer electrolytes and lowered water activity for enlarged potential window. However, the ionic conductivity and mechanical strength of the Na‐ion conducting polymeric gel electrolytes are limited by below 20 mS cm−1 and 2.2 MPa. Herein, we demonstrate Na‐ion conducting and flexible polymeric hydrogel electrolytes of the chemically coupled poly(diallyldimethylammonium chloride)‐dextrin‐N,N′‐methylene‐bis‐acrylamide film immersed in NaClO4 solution (ex‐DDA‐Dex + NaClO4) for flexible sodium‐ion hybrid capacitors (f‐NIHC). In particular, the anion exchange reaction and synergistic interaction of ex‐DDA‐Dex with the optimum ClO4− enable to greatly improve the ionic conductivity up to 27.63 mS cm−1 at 25°C and electrochemical stability window up to 2.6 V, whereas the double networking structure leads to achieve both the mechanical strength (7.48 MPa) and softness of hydrogel electrolytes. Therefore, the f‐NIHCs with the ex‐DDA‐Dex + NaClO4 achieved high specific and high‐rate capacities of 192.04 F g−1 at 500 mA g−1 and 116.06 F g−1 at 10 000 mA g−1, respectively, delivering a large energy density of 120.03 W h kg−1 at 906 W kg−1 and long cyclability of 70% over 500 cycles as well as demonstrating functional operation under mechanical stresses.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139605812","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aluminum–selenium (Al–Se) batteries have been considered as one of the most promising energy storage systems owing to their high capacity, energy density, and cost effectiveness, but Se falls challenges in addressing the shuttle effect of soluble intermediate product and sluggish reaction kinetics in the solid–solid conversion process during cycling. Herein, we propose an unprecedented design concept for fabricating uniform Se/C hollow microspheres with controllable morphologies through low‐temperature electro‐deoxidation in neutral NaCl–AlCl3 molten salt system. Such Se/C hollow microspheres are demonstrated to hold a favorable hollow structure for hosting Se, which can not only suppress the dissolution of soluble intermediate products into the electrolyte, thereby maintaining the structural integrity and maximizing Se utilization of the active material, but also promote the electrical/ionic conductivity, thus facilitating the rapid reaction kinetics during cycling. Accordingly, the as‐prepared Se/C hollow microspheres exhibit a high reversible capacity of 720.1 mAh g−1 at 500 mA g−1. Even at the high current density of 1000 mA g−1, Se/C delivers a high discharge capacity of 564.0 mAh g−1, long‐term stability over 1100 cycles and high Coulombic efficiency of 98.6%. This present work provides valuable insights into short‐process recovery of advanced Se‐containing materials and value‐added utilization for energy storage.
铝硒（Al-Se）电池因其高容量、高能量密度和高成本效益而被认为是最有前途的储能系统之一，但在循环过程中，解决可溶性中间产物的穿梭效应和固-固转换过程中反应动力学迟缓的问题却面临挑战。在此，我们提出了一种前所未有的设计理念，即通过在中性 NaCl-AlCl3 熔盐体系中进行低温电脱氧来制造形态可控的均匀 Se/C 空心微球。实验证明，这种 Se/C 中空微球具有有利于承载 Se 的中空结构，不仅可以抑制可溶性中间产物溶解到电解液中，从而保持结构的完整性，最大限度地提高活性材料的 Se 利用率，还可以提高导电性/离子导电性，从而促进循环过程中的快速反应动力学。因此，制备的 Se/C 空心微球在 500 mA g-1 电流密度下表现出 720.1 mAh g-1 的高可逆容量。即使在 1000 mA g-1 的高电流密度下，Se/C 也能提供 564.0 mAh g-1 的高放电容量、超过 1100 次循环的长期稳定性和 98.6% 的高库仑效率。本研究为先进含硒材料的短流程回收和能源储存的增值利用提供了宝贵的见解。
{"title":"An efficient molten‐salt electro‐deoxidation strategy enabling fast‐kinetics and long‐life aluminum–selenium batteries","authors":"Jiguo Tu, Zheng Huang, Che‐Chiang Chang, Haiping Lei, Shuai Wang, S. Jiao","doi":"10.1002/sus2.183","DOIUrl":"https://doi.org/10.1002/sus2.183","url":null,"abstract":"Aluminum–selenium (Al–Se) batteries have been considered as one of the most promising energy storage systems owing to their high capacity, energy density, and cost effectiveness, but Se falls challenges in addressing the shuttle effect of soluble intermediate product and sluggish reaction kinetics in the solid–solid conversion process during cycling. Herein, we propose an unprecedented design concept for fabricating uniform Se/C hollow microspheres with controllable morphologies through low‐temperature electro‐deoxidation in neutral NaCl–AlCl3 molten salt system. Such Se/C hollow microspheres are demonstrated to hold a favorable hollow structure for hosting Se, which can not only suppress the dissolution of soluble intermediate products into the electrolyte, thereby maintaining the structural integrity and maximizing Se utilization of the active material, but also promote the electrical/ionic conductivity, thus facilitating the rapid reaction kinetics during cycling. Accordingly, the as‐prepared Se/C hollow microspheres exhibit a high reversible capacity of 720.1 mAh g−1 at 500 mA g−1. Even at the high current density of 1000 mA g−1, Se/C delivers a high discharge capacity of 564.0 mAh g−1, long‐term stability over 1100 cycles and high Coulombic efficiency of 98.6%. This present work provides valuable insights into short‐process recovery of advanced Se‐containing materials and value‐added utilization for energy storage.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139606725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Epoxy resins with a high dielectric constant and low intrinsic thermal conductivity coefficient cannot meet the current application requirements of advanced electronic and electrical equipment. Therefore, novel fluorine‐containing liquid crystal epoxy compounds (TFSAEy) with fluorinated groups, biphenyl units, and flexible alkyl chains are first synthesized via amidation and esterification reactions. Then, 4,4′‐diaminodiphenylmethane (DDM) is used as a curing agent to prepare the corresponding fluorine‐containing liquid crystal epoxy resins. The obtained dielectric constant (ε) and dielectric loss (tan δ) values of TFSAEy/DDM at 1 MHz are 2.54 and 0.025, respectively, which are significantly lower than those of conventional epoxy resins (E‐51/DDM, 3.52 and 0.038). Additionally, the intrinsic thermal conductivity coefficient (λ) of TFSAEy/DDM is 0.36 W/(m·K), 71.4% higher than that of E‐51/DDM (0.21 W/(m·K)). Meanwhile, the corresponding elastic modulus, hardness, glass transition temperature, and heat resistance index of TFSAEy/DDM are 5.73 GPa, 0.35 GPa, 213.5°C, and 188.7°C, respectively, all superior to those of E‐51/DDM (3.68 GPa, 0.27 GPa, 107.2°C, and 174.8°C), presenting potential application in high‐heating electronic component packaging and printed circuit boards.
{"title":"Low dielectric constant and highly intrinsic thermal conductivity fluorine‐containing epoxy resins with ordered liquid crystal structures","authors":"Xuerong Fan, Zheng Liu, Shuangshuang Wang, Junwei Gu","doi":"10.1002/sus2.172","DOIUrl":"https://doi.org/10.1002/sus2.172","url":null,"abstract":"Epoxy resins with a high dielectric constant and low intrinsic thermal conductivity coefficient cannot meet the current application requirements of advanced electronic and electrical equipment. Therefore, novel fluorine‐containing liquid crystal epoxy compounds (TFSAEy) with fluorinated groups, biphenyl units, and flexible alkyl chains are first synthesized via amidation and esterification reactions. Then, 4,4′‐diaminodiphenylmethane (DDM) is used as a curing agent to prepare the corresponding fluorine‐containing liquid crystal epoxy resins. The obtained dielectric constant (ε) and dielectric loss (tan δ) values of TFSAEy/DDM at 1 MHz are 2.54 and 0.025, respectively, which are significantly lower than those of conventional epoxy resins (E‐51/DDM, 3.52 and 0.038). Additionally, the intrinsic thermal conductivity coefficient (λ) of TFSAEy/DDM is 0.36 W/(m·K), 71.4% higher than that of E‐51/DDM (0.21 W/(m·K)). Meanwhile, the corresponding elastic modulus, hardness, glass transition temperature, and heat resistance index of TFSAEy/DDM are 5.73 GPa, 0.35 GPa, 213.5°C, and 188.7°C, respectively, all superior to those of E‐51/DDM (3.68 GPa, 0.27 GPa, 107.2°C, and 174.8°C), presenting potential application in high‐heating electronic component packaging and printed circuit boards.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138592488","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Jiang, Xu Wu, Heng Zhang, Qiong Yan, Hui Li, Tianyi Ma, Song Yang
Thermochemical conversion of fossil resources into fuels, chemicals, and materials has rapidly increased atmospheric CO2 levels, hindering global efforts toward achieving carbon neutrality. With the increasing push for sustainability, utilizing electrochemical technology to transform CO2 or biomass into value‐added chemicals and to close the carbon cycle with sustainable energy sources represents a promising strategy. Expanding the scope of electrosynthesis technology is a prerequisite for the electrification of chemical manufacturing. To this end, constructing the C─N bond is considered a priority. However, a systematic review of electrocatalytic processes toward building C─N bonds using CO2 and biomass as carbon sources is not available. Accordingly, this review highlights the research progress in the electrosynthesis of organic nitrogen compounds from CO2 and biomass by C─N coupling reactions in view of catalytic materials, focusing on the enlightenment of traditional catalysis on C─N coupling and the understanding of the basis of electrochemical C─N coupling. The possibility of C─N bond in electrocatalysis is also examined from the standpoints of activation of substrates, coupling site, mechanism, and inhibition of hydrogen evolution reaction (HER). Finally, the challenges and prospects of electrocatalytic C─N coupling reactions with improved efficiency and selectivity for future development are discussed.
{"title":"Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO2 and biomass as carbon sources","authors":"Hao Jiang, Xu Wu, Heng Zhang, Qiong Yan, Hui Li, Tianyi Ma, Song Yang","doi":"10.1002/sus2.175","DOIUrl":"https://doi.org/10.1002/sus2.175","url":null,"abstract":"Thermochemical conversion of fossil resources into fuels, chemicals, and materials has rapidly increased atmospheric CO2 levels, hindering global efforts toward achieving carbon neutrality. With the increasing push for sustainability, utilizing electrochemical technology to transform CO2 or biomass into value‐added chemicals and to close the carbon cycle with sustainable energy sources represents a promising strategy. Expanding the scope of electrosynthesis technology is a prerequisite for the electrification of chemical manufacturing. To this end, constructing the C─N bond is considered a priority. However, a systematic review of electrocatalytic processes toward building C─N bonds using CO2 and biomass as carbon sources is not available. Accordingly, this review highlights the research progress in the electrosynthesis of organic nitrogen compounds from CO2 and biomass by C─N coupling reactions in view of catalytic materials, focusing on the enlightenment of traditional catalysis on C─N coupling and the understanding of the basis of electrochemical C─N coupling. The possibility of C─N bond in electrocatalysis is also examined from the standpoints of activation of substrates, coupling site, mechanism, and inhibition of hydrogen evolution reaction (HER). Finally, the challenges and prospects of electrocatalytic C─N coupling reactions with improved efficiency and selectivity for future development are discussed.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139017880","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Cesium lead triiodide (CsPbI3) perovskite receives tremendous attention for photovoltaic applications, owing to its remarkable thermal stability and optoelectronic properties. However, realizing the CsPbI3 perovskite with high black‐phase stability and optoelectronic properties remains a significant challenge, which largely affects the photovoltaic performance of perovskite solar cells (PSCs). Herein, aromatic ammonium agents are used to modulate the crystallization of the CsPbI3 perovskite to improve its black‐phase stability and optoelectronic properties for efficient PSCs. Systemically experimental studies and comprehensively theoretical calculations are performed, which reveal that histammonium dihydrochloride (HACl2) could strongly couple with the perovskite during its crystallization, leading to faster nucleation and slower perovskite growth, and thus modulating the crystallization dynamics of the perovskites. Moreover, the residual diammonium cations (HA2+) distributed at the grain boundaries and on the surface of the perovskites can effectively passivate defects through electrostatic interactions, substantially suppressing trap‐assisted nonradiative recombination, and prompting more matched perovskite surface energetics. Consequently, the photovoltaic performance of CsPbI3 PSCs is largely improved because of a combination of enhanced crystallinity and optoelectronic properties of the perovskites. This work offers a new avenue to prepare inorganic perovskites with high optoelectronic properties for photovoltaics.
{"title":"Modulating CsPbl3 crystallization by using diammonium agent for efficient solar cells","authors":"Junming Qiu, Qisen Zhou, Mei Yu, Jianhua Liu, Rongshan Zhuang, Yong Hua, Liming Ding, Xiaoliang Zhang","doi":"10.1002/sus2.173","DOIUrl":"https://doi.org/10.1002/sus2.173","url":null,"abstract":"Cesium lead triiodide (CsPbI3) perovskite receives tremendous attention for photovoltaic applications, owing to its remarkable thermal stability and optoelectronic properties. However, realizing the CsPbI3 perovskite with high black‐phase stability and optoelectronic properties remains a significant challenge, which largely affects the photovoltaic performance of perovskite solar cells (PSCs). Herein, aromatic ammonium agents are used to modulate the crystallization of the CsPbI3 perovskite to improve its black‐phase stability and optoelectronic properties for efficient PSCs. Systemically experimental studies and comprehensively theoretical calculations are performed, which reveal that histammonium dihydrochloride (HACl2) could strongly couple with the perovskite during its crystallization, leading to faster nucleation and slower perovskite growth, and thus modulating the crystallization dynamics of the perovskites. Moreover, the residual diammonium cations (HA2+) distributed at the grain boundaries and on the surface of the perovskites can effectively passivate defects through electrostatic interactions, substantially suppressing trap‐assisted nonradiative recombination, and prompting more matched perovskite surface energetics. Consequently, the photovoltaic performance of CsPbI3 PSCs is largely improved because of a combination of enhanced crystallinity and optoelectronic properties of the perovskites. This work offers a new avenue to prepare inorganic perovskites with high optoelectronic properties for photovoltaics.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139013439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Siwei Fan, Yijie Liu, Yun Gao, Yang Liu, Yun Qiao, Li Li, Shu‐Lei Chou
Sodium‐ion batteries (SIBs) present great appeal in various energy storage systems, especifically for stationary grid storage, on account of the abundance of sources and low cost. Unfortunately, the commercialization of SIBs is mainly limited by available electrode materials, especially for the cathodes. Prussian blue analogs (PBAs), emerge as a promising alternative for their structural feasibility in the application of SIBs. Decreasing the defects (vacancies and coordinated water) is an effective strategy to achieve superior electrochemical performance during the synthetic processes. Herein, we summarize crystal structures, synthetic methods, electrochemical mechanisms, and the influences of synthesis conditions of PBAs in detail. This comprehensive overview on the current research progresses of PBAs will give guides and directions to solve the existing problems for their application in SIBs.
{"title":"The design and synthesis of Prussian blue analogs as a sustainable cathode for sodium‐ion batteries","authors":"Siwei Fan, Yijie Liu, Yun Gao, Yang Liu, Yun Qiao, Li Li, Shu‐Lei Chou","doi":"10.1002/sus2.170","DOIUrl":"https://doi.org/10.1002/sus2.170","url":null,"abstract":"Sodium‐ion batteries (SIBs) present great appeal in various energy storage systems, especifically for stationary grid storage, on account of the abundance of sources and low cost. Unfortunately, the commercialization of SIBs is mainly limited by available electrode materials, especially for the cathodes. Prussian blue analogs (PBAs), emerge as a promising alternative for their structural feasibility in the application of SIBs. Decreasing the defects (vacancies and coordinated water) is an effective strategy to achieve superior electrochemical performance during the synthetic processes. Herein, we summarize crystal structures, synthetic methods, electrochemical mechanisms, and the influences of synthesis conditions of PBAs in detail. This comprehensive overview on the current research progresses of PBAs will give guides and directions to solve the existing problems for their application in SIBs.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139013303","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abstract Covalent organic frameworks (COFs) have been developed as the precursors to construct porous carbons for electrocatalytic systems. However, the influences of carbon dimensions on the catalytic performance are still underexplored. In this work, we have first constructed COF‐derived carbons by template‐synthesis strategy in different dimensions to catalyze the carbon dioxide reduction (CO 2 RR). By using different templates, the one‐dimensional (1D), two‐dimensional (2D), and three‐dimensional (3D) COF‐derived carbons have been employed to anchor Co‐porphyrin to form the Co‐N 5 sites to catalyze CO 2 RR. The 1D catalyst templated by carbon nano tubes presents high binding ability of CO 2 , more defective sites, and higher electronic conductivity, resulting in a higher catalytic activity for CO 2 and selectivity of CO than 2D and 3D carbon‐based catalysts. The 1D catalyst delivers the turnover frequency values of 1150 h −1 and the FECO of 94.5% at 0.7 V versus RHE, which is significantly better than those of 2D and 3D carbon‐based catalysts.
{"title":"Dimensional engineering of covalent organic frameworks derived carbons for electrocatalytic carbon dioxide reduction","authors":"Guojuan Liu, Xuewen Li, Minghao Liu, Xiubei Yang, Zhuangyan Guo, Xinqing Chen, Qing Xu, Gaofeng Zeng, Yue He","doi":"10.1002/sus2.167","DOIUrl":"https://doi.org/10.1002/sus2.167","url":null,"abstract":"Abstract Covalent organic frameworks (COFs) have been developed as the precursors to construct porous carbons for electrocatalytic systems. However, the influences of carbon dimensions on the catalytic performance are still underexplored. In this work, we have first constructed COF‐derived carbons by template‐synthesis strategy in different dimensions to catalyze the carbon dioxide reduction (CO 2 RR). By using different templates, the one‐dimensional (1D), two‐dimensional (2D), and three‐dimensional (3D) COF‐derived carbons have been employed to anchor Co‐porphyrin to form the Co‐N 5 sites to catalyze CO 2 RR. The 1D catalyst templated by carbon nano tubes presents high binding ability of CO 2 , more defective sites, and higher electronic conductivity, resulting in a higher catalytic activity for CO 2 and selectivity of CO than 2D and 3D carbon‐based catalysts. The 1D catalyst delivers the turnover frequency values of 1150 h −1 and the FECO of 94.5% at 0.7 V versus RHE, which is significantly better than those of 2D and 3D carbon‐based catalysts.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135292237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yiming Zhang, Weiqiong Zheng, Huijuan Wu, Ran Zhu, Yinghan Wang, Mao Wang, Tian Ma, Chong Cheng, Zhiyuan Zeng, Shuang Li
Abstract Ruthenium (Ru) has been recognized as a prospective candidate to substitute platinum catalysts in water‐splitting‐based hydrogen production. However, minimizing the Ru contents, optimizing the water dissociation energy of Ru sites, and enhancing the long‐term stability are extremely required, but still face a great challenge. Here, we report on creating tungsten oxide‐anchored Ru clusters (Ru–WO x ) with electron‐rich and anti‐corrosive microenvironments for efficient and robust seawater splitting. Benefiting from the abundant oxygen vacancy structure in tungsten oxide support, the Ru–WO x exhibits strong Ru–O and Ru–W bonds at the interface. Our study elucidates that the strong Ru–O bonds in Ru–WO x may accelerate the water dissociation kinetics, and the Ru–W bonds will lead to the strong metal–support interaction and electrons transfer from W to Ru. The optimal Ru–WO x catalysts exhibit a low overpotential of 29 and 218 mV at the current density of 10 mA cm −2 in alkaline and seawater media, respectively. The outstanding long‐term stability discloses that the Ru–WO x catalysts own efficient corrosion resistance in seawater electrolysis. We believe that this work offers new insights into the essential roles of electron‐rich and anti‐corrosive microenvironments in Ru‐based catalysts and provide a new pathway to design efficient and robust cathodes for seawater splitting.
摘要钌(Ru)已被认为是替代铂催化剂在水裂解制氢中的潜在候选催化剂。然而，降低Ru含量，优化Ru位点的水解离能，提高长期稳定性是迫切需要的，但仍然面临着很大的挑战。在这里，我们报道了在富电子和抗腐蚀的微环境中创建氧化钨锚定的Ru团簇(Ru - wo x)，用于高效和强大的海水分裂。得益于氧化钨载体中丰富的氧空位结构，Ru-WO - x在界面处表现出很强的Ru-O和Ru-W键。我们的研究表明，Ru - wo x中的强Ru - o键可能会加速水的解离动力学，而Ru - W键会导致强金属支撑相互作用和电子从W转移到Ru。在碱性介质和海水介质中，当电流密度为10 mA cm−2时，Ru-WO - x催化剂的过电位分别为29 mV和218 mV。优异的长期稳定性表明Ru-WO - x催化剂在海水电解中具有良好的耐腐蚀性。我们相信这项工作为富电子和抗腐蚀微环境在钌基催化剂中的重要作用提供了新的见解，并为设计高效和坚固的海水分裂阴极提供了新的途径。
{"title":"Tungsten oxide‐anchored Ru clusters with electron‐rich and anti‐corrosive microenvironments for efficient and robust seawater splitting","authors":"Yiming Zhang, Weiqiong Zheng, Huijuan Wu, Ran Zhu, Yinghan Wang, Mao Wang, Tian Ma, Chong Cheng, Zhiyuan Zeng, Shuang Li","doi":"10.1002/sus2.164","DOIUrl":"https://doi.org/10.1002/sus2.164","url":null,"abstract":"Abstract Ruthenium (Ru) has been recognized as a prospective candidate to substitute platinum catalysts in water‐splitting‐based hydrogen production. However, minimizing the Ru contents, optimizing the water dissociation energy of Ru sites, and enhancing the long‐term stability are extremely required, but still face a great challenge. Here, we report on creating tungsten oxide‐anchored Ru clusters (Ru–WO x ) with electron‐rich and anti‐corrosive microenvironments for efficient and robust seawater splitting. Benefiting from the abundant oxygen vacancy structure in tungsten oxide support, the Ru–WO x exhibits strong Ru–O and Ru–W bonds at the interface. Our study elucidates that the strong Ru–O bonds in Ru–WO x may accelerate the water dissociation kinetics, and the Ru–W bonds will lead to the strong metal–support interaction and electrons transfer from W to Ru. The optimal Ru–WO x catalysts exhibit a low overpotential of 29 and 218 mV at the current density of 10 mA cm −2 in alkaline and seawater media, respectively. The outstanding long‐term stability discloses that the Ru–WO x catalysts own efficient corrosion resistance in seawater electrolysis. We believe that this work offers new insights into the essential roles of electron‐rich and anti‐corrosive microenvironments in Ru‐based catalysts and provide a new pathway to design efficient and robust cathodes for seawater splitting.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135778868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jihyun Kim, Sang‐Won Park, Younghyun Lee, Hideo Hosono, Byungwoo Park, Jinhyun Kim
As a next‐generation photovoltaic device, perovskite solar cells are rapidly emerging. Nevertheless, both solution and device stability pose challenges for commercialization due to chemical degradation caused by internal and external factors. Especially, the decomposition of iodoplumbate in a perovskite solution hinders the long‐term use of perovskite solutions. Moreover, the synthesis of stable perovskites at low temperature is important for stable devices and wide applications (flexible devices and high reproducibility). Herein, the critical composition of perovskite is found to obtain high stabilities of both iodoplumbate and perovskite crystals by utilizing CsPbBr3 and FAPbI3, exhibiting high device performance and long‐term solution storage. The novel composition of CsPbBr3‐alloyed FAPbI3 not only crystallizes under annealing‐free conditions but also demonstrates excellent iodoplumbate stability for 100 days (∼3000 h) without any degradation. Furthermore, high device stabilities are achieved over 2000 and 3000 h under extreme conditions of A.M. 1.5 and 85°C/85% relative humidity, respectively. Overall, the device exhibited a high power conversion efficiency of 23.4%, and furthermore, CsPbBr3‐alloyed FAPbI3 was devoted to widen the applications in both flexible and carbon‐electrode devices, thereby addressing both scientific depths and potential commercial materials.
{"title":"Synthesis of stable iodoplumbate and perovskite for efficient annealing‐free device and long‐term storage","authors":"Jihyun Kim, Sang‐Won Park, Younghyun Lee, Hideo Hosono, Byungwoo Park, Jinhyun Kim","doi":"10.1002/sus2.163","DOIUrl":"https://doi.org/10.1002/sus2.163","url":null,"abstract":"As a next‐generation photovoltaic device, perovskite solar cells are rapidly emerging. Nevertheless, both solution and device stability pose challenges for commercialization due to chemical degradation caused by internal and external factors. Especially, the decomposition of iodoplumbate in a perovskite solution hinders the long‐term use of perovskite solutions. Moreover, the synthesis of stable perovskites at low temperature is important for stable devices and wide applications (flexible devices and high reproducibility). Herein, the critical composition of perovskite is found to obtain high stabilities of both iodoplumbate and perovskite crystals by utilizing CsPbBr3 and FAPbI3, exhibiting high device performance and long‐term solution storage. The novel composition of CsPbBr3‐alloyed FAPbI3 not only crystallizes under annealing‐free conditions but also demonstrates excellent iodoplumbate stability for 100 days (∼3000 h) without any degradation. Furthermore, high device stabilities are achieved over 2000 and 3000 h under extreme conditions of A.M. 1.5 and 85°C/85% relative humidity, respectively. Overall, the device exhibited a high power conversion efficiency of 23.4%, and furthermore, CsPbBr3‐alloyed FAPbI3 was devoted to widen the applications in both flexible and carbon‐electrode devices, thereby addressing both scientific depths and potential commercial materials.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136037920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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