Cuprous oxide (Cu2O) as an intrinsic p-type semiconductor is promising for solar energy conversion. The major challenge in fabricating Cu2O lies in achieving both high transparency and high performance in a tandem device. The Cu2O photocathodes often employ gold as the back contact layer. However, it is not an optimal choice in tandem device due to its poor transmission, scarcity, and electron-hole recombination at the interface of Au and Cu2O. Here, we presented a facile method that utilizes the earth-abundant material copper oxide (CuO) to fabricate highly transparent Cu2O devices. The maximum transmittance of the Cu2O film on CuO (FTO/CuO/Cu2O) increased from 42 % to 58 % compared with Cu2O film on Au (FTO/Au (3 nm)/Cu2O) in 550-800 nm. After coating atomic layer deposition (ALD) layers and hydrogen evolution reaction (HER) catalyst, the photocurrent density at 0 V (versus RHE) of the semitransparent Cu2O photocathode with CuO as the back layer for photoelectrochemical (PEC) water splitting reached -4.9 mA cm-2, which showed a 24.5 % improvement compared with FTO/Au/Cu2O photocathode. Moreover, expanding the CuO layer strategy to the field of solar cells enables Cu2O solar cells to achieve a PCE of 2.37 %.
{"title":"Semitransparent Cu<sub>2</sub>O Films Based on CuO Back Layer for Photoelectrochemical Water Splitting and Photovoltaic Applications.","authors":"Linxiao Wu, Jinshui Cheng, Jingshan Luo","doi":"10.1002/cssc.202401994","DOIUrl":"10.1002/cssc.202401994","url":null,"abstract":"<p><p>Cuprous oxide (Cu<sub>2</sub>O) as an intrinsic p-type semiconductor is promising for solar energy conversion. The major challenge in fabricating Cu<sub>2</sub>O lies in achieving both high transparency and high performance in a tandem device. The Cu<sub>2</sub>O photocathodes often employ gold as the back contact layer. However, it is not an optimal choice in tandem device due to its poor transmission, scarcity, and electron-hole recombination at the interface of Au and Cu<sub>2</sub>O. Here, we presented a facile method that utilizes the earth-abundant material copper oxide (CuO) to fabricate highly transparent Cu<sub>2</sub>O devices. The maximum transmittance of the Cu<sub>2</sub>O film on CuO (FTO/CuO/Cu<sub>2</sub>O) increased from 42 % to 58 % compared with Cu<sub>2</sub>O film on Au (FTO/Au (3 nm)/Cu<sub>2</sub>O) in 550-800 nm. After coating atomic layer deposition (ALD) layers and hydrogen evolution reaction (HER) catalyst, the photocurrent density at 0 V (versus RHE) of the semitransparent Cu<sub>2</sub>O photocathode with CuO as the back layer for photoelectrochemical (PEC) water splitting reached -4.9 mA cm<sup>-2</sup>, which showed a 24.5 % improvement compared with FTO/Au/Cu<sub>2</sub>O photocathode. Moreover, expanding the CuO layer strategy to the field of solar cells enables Cu<sub>2</sub>O solar cells to achieve a PCE of 2.37 %.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401994"},"PeriodicalIF":7.5,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491609","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lizi He, Ning Han, Zirui Lang, Meiyang Wang, Yuqin Wang, Lishuang Li
Aluminum-air battery has the advantages of high energy density, low cost and environmental protection, and is considered as an ideal next-generation energy storage conversion system. However, the slow oxygen reduction reaction (ORR) in air cathode leads to its unsatisfactory performance. Here, we report an electrode made of N and Ni co-doped MnO2 nanotubes. In alkaline solution, Ni/N-MnO2 has higher oxygen reduction activity than undoped MnO2, with an initial potential of 1.00 V and a half-wave potential of 0.75 V. This is because it has abundant defects, high specific surface area and sufficient Mn3+ active sites, which promote the transfer of electrons and oxygen-containing intermediates. Density functional theory (DFT) calculations show that MnO2 doped with N and Ni atoms reduces the reaction overpotential and improves the ORR kinetics. The peak power density and energy density of the Ni/N-MnO2 air electrode increased by 34.03 mW cm-2 and 316.41 mWh g-1, respectively. The results show that N and Ni co-doped MnO2 nanotubes are a promising air electrode, which can provide some ideas for the research of aluminum-air batteries.
铝空气电池具有能量密度高、成本低和环保等优点,被认为是理想的下一代储能转换系统。然而,空气阴极中缓慢的氧还原反应(ORR)导致其性能不尽如人意。在此,我们报告了一种由 N 和 Ni 共掺杂的 MnO2 纳米管制成的电极。在碱性溶液中,Ni/N-MnO2 比未掺杂的 MnO2 具有更高的氧还原活性,初始电位为 1.00 V,半波电位为 0.75 V,这是因为它具有丰富的缺陷、高比表面积和足够的 Mn3+ 活性位点,这些都促进了电子和含氧中间产物的转移。密度泛函理论(DFT)计算表明,掺杂 N 原子和 Ni 原子的 MnO2 可降低反应过电位,改善 ORR 动力学。Ni/N-MnO2 空气电极的峰值功率密度和能量密度分别增加了 34.03 mW-cm-2 和 316.41 mWh-g-1。结果表明,N和Ni共掺杂的MnO2纳米管是一种很有前景的空气电极,可为铝空气电池的研究提供一些思路。
{"title":"Nickel-Nitrogen Doped MnO<sub>2</sub> as Oxygen Reduction Reaction Catalyst for Aluminum Air Batteries.","authors":"Lizi He, Ning Han, Zirui Lang, Meiyang Wang, Yuqin Wang, Lishuang Li","doi":"10.1002/cssc.202401385","DOIUrl":"10.1002/cssc.202401385","url":null,"abstract":"<p><p>Aluminum-air battery has the advantages of high energy density, low cost and environmental protection, and is considered as an ideal next-generation energy storage conversion system. However, the slow oxygen reduction reaction (ORR) in air cathode leads to its unsatisfactory performance. Here, we report an electrode made of N and Ni co-doped MnO<sub>2</sub> nanotubes. In alkaline solution, Ni/N-MnO<sub>2</sub> has higher oxygen reduction activity than undoped MnO<sub>2</sub>, with an initial potential of 1.00 V and a half-wave potential of 0.75 V. This is because it has abundant defects, high specific surface area and sufficient Mn<sup>3+</sup> active sites, which promote the transfer of electrons and oxygen-containing intermediates. Density functional theory (DFT) calculations show that MnO<sub>2</sub> doped with N and Ni atoms reduces the reaction overpotential and improves the ORR kinetics. The peak power density and energy density of the Ni/N-MnO<sub>2</sub> air electrode increased by 34.03 mW cm<sup>-2</sup> and 316.41 mWh g<sup>-1</sup>, respectively. The results show that N and Ni co-doped MnO<sub>2</sub> nanotubes are a promising air electrode, which can provide some ideas for the research of aluminum-air batteries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401385"},"PeriodicalIF":7.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491606","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Seonjeong Cheon, Beomseo Kim, Hyun-Woo Kim, DongYeon Kim, Jong-In Han
The electrochemical reduction of nitric oxide (NO) to ammonia (NH3) offers a sustainable way of simultaneously treating the air pollutant and producing a useful chemical. Among catalyst candidates, Cu emerges as a stand-out choice for its superb NH3 selectivity and production rate. However, a comprehensive study concerning its catalytic behavior in the NO reduction environment is still lacking. Here, we unravel the dynamic rearrangement of Cu catalysts during NO reduction: the emergence of a bundled nanowire structure dependent on the applied potential. This unique structure is closely linked to an enhancement in double-layer capacitance, leading to a progressive increase in current density from 236 mA cm-2 by 20 % over 1 h, while maintaining a Faradaic efficiency of 95 % for NH3. Characterizations of Cu oxidation states suggest that the nanostructure results from the dissolution-redeposition of Cu in the aqueous electrolyte, influenced by the interaction with NO or other reactive intermediates. This understanding contributes to the broader exploration of Cu-based catalysts for sustainable and efficient NH3 synthesis from NO.
将一氧化氮(NO)电化学还原成氨气(NH3)是同时处理空气污染物和生产有用化学品的一种可持续方法。在候选催化剂中,铜因其出色的 NH3 选择性和生产率而脱颖而出。然而,有关其在氮氧化物还原环境中的催化行为的全面研究还很缺乏。在此,我们揭示了铜催化剂在氮氧化物还原过程中的动态重排:出现了一种取决于外加电势的束状纳米线结构。这种独特的结构与双层电容的增强密切相关,导致电流密度在 1 小时内从 236 mA cm-2 逐步增加 20%,同时对 NH3 的法拉第效率保持在 95%。对铜氧化态的表征表明,纳米结构是铜在水性电解质中溶解-再沉积的结果,受到与 NO 或其他反应性中间产物相互作用的影响。这一认识有助于对铜基催化剂进行更广泛的探索,以实现从 NO 到 NH3 的可持续高效合成。
{"title":"Dynamic Reconstruction of Cu Catalyst Under Electrochemical NO Reduction to NH<sub>3</sub>.","authors":"Seonjeong Cheon, Beomseo Kim, Hyun-Woo Kim, DongYeon Kim, Jong-In Han","doi":"10.1002/cssc.202401978","DOIUrl":"10.1002/cssc.202401978","url":null,"abstract":"<p><p>The electrochemical reduction of nitric oxide (NO) to ammonia (NH<sub>3</sub>) offers a sustainable way of simultaneously treating the air pollutant and producing a useful chemical. Among catalyst candidates, Cu emerges as a stand-out choice for its superb NH<sub>3</sub> selectivity and production rate. However, a comprehensive study concerning its catalytic behavior in the NO reduction environment is still lacking. Here, we unravel the dynamic rearrangement of Cu catalysts during NO reduction: the emergence of a bundled nanowire structure dependent on the applied potential. This unique structure is closely linked to an enhancement in double-layer capacitance, leading to a progressive increase in current density from 236 mA cm<sup>-2</sup> by 20 % over 1 h, while maintaining a Faradaic efficiency of 95 % for NH<sub>3</sub>. Characterizations of Cu oxidation states suggest that the nanostructure results from the dissolution-redeposition of Cu in the aqueous electrolyte, influenced by the interaction with NO or other reactive intermediates. This understanding contributes to the broader exploration of Cu-based catalysts for sustainable and efficient NH<sub>3</sub> synthesis from NO.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401978"},"PeriodicalIF":7.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491594","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Reasonably screening the targeted oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) constituents and constructing high-efficiency and stabilized ORR/OER bifunctional electrocatalysts are pivotal for the advancement of rechargeable zinc-air batteries (ZABs). Here, CoFe layered double hydroxide (CoFe-LDH) nanosheets are deposited on nitrogen-doped graphite-carbon polyhedra with FeCo alloy nanoparticles (FeCo/LDH-NGCP). Due to the synergic effect between FeCo-NGCP, CoFe-LDH and FeCo/LDH-NGCP, the electrocatalyst with the abundant and accessible active sites can provide good charge/mass transfer, and thus shows wonderful ORR and OER bifunctional electrocatalytic performance. In ORR tests, FeCo/LDH-NGCP catalyst displays larger half-wave potential (E1/2, 0.89 V vs. 0.85 V), higher limiting current density (JL, 5.91 mA/cm2 vs. 5.14 mA/cm2) and better stability than commercial Pt/C. As for OER, FeCo/LDH-NGCP possesses a smaller overpotential (η) of 299.6 mV at a current density of 10 mA/cm2 and more durable stability than commercial RuO2 (330.6 mV). Furthermore, in ZAB tests, the cycling stability of ZAB-FeCo/LDH-NGCP (over 470 h) outperforms the ZAB-Pt/C+RuO2 (92 h) with commercial electrocatalyst (Pt/C+RuO2). Therefore, the FeCo/LDH-NGCP catalyst offers a new perspective to construct ZABs bifunctional catalysts and their commercial application in ZABs.
{"title":"FeCo Bimetallic ZIF Derivatives Decorated with CoFe-LDH to Promote Bifunctional Oxygen Electrocatalysis Activation.","authors":"Feng Zhang, Yu Lei, Guang Li, Yangchen Xie, Xinjia Guo, Xiaoyan Zhang, Xianyou Wang","doi":"10.1002/cssc.202401556","DOIUrl":"10.1002/cssc.202401556","url":null,"abstract":"<p><p>Reasonably screening the targeted oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) constituents and constructing high-efficiency and stabilized ORR/OER bifunctional electrocatalysts are pivotal for the advancement of rechargeable zinc-air batteries (ZABs). Here, CoFe layered double hydroxide (CoFe-LDH) nanosheets are deposited on nitrogen-doped graphite-carbon polyhedra with FeCo alloy nanoparticles (FeCo/LDH-NGCP). Due to the synergic effect between FeCo-NGCP, CoFe-LDH and FeCo/LDH-NGCP, the electrocatalyst with the abundant and accessible active sites can provide good charge/mass transfer, and thus shows wonderful ORR and OER bifunctional electrocatalytic performance. In ORR tests, FeCo/LDH-NGCP catalyst displays larger half-wave potential (E<sub>1/2</sub>, 0.89 V vs. 0.85 V), higher limiting current density (J<sub>L</sub>, 5.91 mA/cm<sup>2</sup> vs. 5.14 mA/cm<sup>2</sup>) and better stability than commercial Pt/C. As for OER, FeCo/LDH-NGCP possesses a smaller overpotential (η) of 299.6 mV at a current density of 10 mA/cm<sup>2</sup> and more durable stability than commercial RuO<sub>2</sub> (330.6 mV). Furthermore, in ZAB tests, the cycling stability of ZAB-FeCo/LDH-NGCP (over 470 h) outperforms the ZAB-Pt/C+RuO<sub>2</sub> (92 h) with commercial electrocatalyst (Pt/C+RuO<sub>2</sub>). Therefore, the FeCo/LDH-NGCP catalyst offers a new perspective to construct ZABs bifunctional catalysts and their commercial application in ZABs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401556"},"PeriodicalIF":7.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuke Su, Suqin Liu, Weiwei Zhu, Kui Huang, Da Huang, Peng Jiang, Jianhui Liu, Guang Yang, Zhen He, Jue Wang
The tightly bonded structure of polybenzimidazole (PBI) membrane is the origin of its poor proton conductivity, which severely hinders achieving a cost-effective membrane for vanadium redox flow battery (VRFB). It desires a strategy to relax the membrane structure to significantly improve the proton conductivity and maintain its structure stability. Therefore, this work proposes a novel strategy through regulating molecular interactions within PBI membrane to loosen up the structure of PBI membrane and dramatically enhance the proton conductivity. The interactions in PBI membrane are switched by DMSO/water and acid through sequentially treating membrane with these solutions. The efficient PBI membrane prepared using this strategy demonstrates an outstanding performance for VRFB, with the proton conductivity enhanced by 3850 % (from 1.9 to 76.3 mS cm-1), and VRFB achieves a high energy efficiency of 80.5 % under 200 mA cm-2. More importantly, this work shed lights on the structure-property relationship of PBI membrane, and the mechanism in enhancing proton conductivity is unraveled, which is of great significance for the development of VRFB membranes.
聚苯并咪唑(PBI)膜的紧键结构是其质子传导性差的根源,这严重阻碍了钒氧化还原液流电池(VRFB)膜成本效益的实现。这就需要一种放松膜结构的策略,以显著提高质子传导性并保持其结构稳定性。因此,本研究提出了一种新策略,通过调节 PBI 膜内的分子相互作用来松弛 PBI 膜的结构,从而显著提高质子传导性。通过用二甲基亚砜/水和酸依次处理 PBI 膜,可以切换膜内的相互作用。利用这种策略制备的高效 PBI 膜在 VRFB 上表现出了卓越的性能,质子电导率提高了 3850%(从 1.9 mS cm-1 提高到 76.3 mS cm-1),VRFB 在 200 mA cm-2 下实现了 80.5% 的高能效。更重要的是,该研究揭示了 PBI 膜的结构-性能关系,揭示了质子传导性增强的机理,对 VRFB 膜的开发具有重要意义。
{"title":"Regulating Molecular Interactions in Polybenzimidazole Membrane for Efficient Vanadium Redox Flow Battery.","authors":"Yuke Su, Suqin Liu, Weiwei Zhu, Kui Huang, Da Huang, Peng Jiang, Jianhui Liu, Guang Yang, Zhen He, Jue Wang","doi":"10.1002/cssc.202401576","DOIUrl":"10.1002/cssc.202401576","url":null,"abstract":"<p><p>The tightly bonded structure of polybenzimidazole (PBI) membrane is the origin of its poor proton conductivity, which severely hinders achieving a cost-effective membrane for vanadium redox flow battery (VRFB). It desires a strategy to relax the membrane structure to significantly improve the proton conductivity and maintain its structure stability. Therefore, this work proposes a novel strategy through regulating molecular interactions within PBI membrane to loosen up the structure of PBI membrane and dramatically enhance the proton conductivity. The interactions in PBI membrane are switched by DMSO/water and acid through sequentially treating membrane with these solutions. The efficient PBI membrane prepared using this strategy demonstrates an outstanding performance for VRFB, with the proton conductivity enhanced by 3850 % (from 1.9 to 76.3 mS cm<sup>-1</sup>), and VRFB achieves a high energy efficiency of 80.5 % under 200 mA cm<sup>-2</sup>. More importantly, this work shed lights on the structure-property relationship of PBI membrane, and the mechanism in enhancing proton conductivity is unraveled, which is of great significance for the development of VRFB membranes.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401576"},"PeriodicalIF":7.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491608","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Boosting the energy and power densities of electrochemical energy storage (EES) devices to broaden their practicality is of great significance and emergently desirable. Recently, the EES cells with an anode-free concept have been announced to realize those targets. Herein, 20 μm of a zincophilic layer prepared by blending ZIF-8 and sodium alginate (SA) is uniformly coated on Cu foil (Z8-SA@Cu) as an alternative anode for anode-less zinc-ion hybrid supercapacitors (ALZHSCs). Contributing by the distinctive features evidenced by electrochemical measurements and post-mortem analyses: (1) less nucleation barrier and overpotential, (2) limited zincate formation, (3) improved Zn2+ flux and (4) efficient Zn plating/stripping, the as-prepared Z8-SA@Cu is rationally considered to be a promising anode for ALZHSCs. Encouragingly, the assembled ALZHSC device not only delivers an impressive rate capability (40 mAh/g at 1 mA/cm2 and 34 mAh/g at 10 mA/cm2) but also achieves the excellent cycling stability (capacity retention: 88 % after 12,000 cycles at 5 mA). Most importantly, the ALZHSC device also reveals significant increases in gravimetric energy density and high-power ability as compared to the traditional ZHSCs.
{"title":"Win-Win Strategies Enable Efficient Anode-Less Zinc-Ion Hybrid Supercapacitors.","authors":"Tai-Feng Hung, Rene Mary Amirtha, Chun-Chen Yang","doi":"10.1002/cssc.202402140","DOIUrl":"10.1002/cssc.202402140","url":null,"abstract":"<p><p>Boosting the energy and power densities of electrochemical energy storage (EES) devices to broaden their practicality is of great significance and emergently desirable. Recently, the EES cells with an anode-free concept have been announced to realize those targets. Herein, 20 μm of a zincophilic layer prepared by blending ZIF-8 and sodium alginate (SA) is uniformly coated on Cu foil (Z8-SA@Cu) as an alternative anode for anode-less zinc-ion hybrid supercapacitors (ALZHSCs). Contributing by the distinctive features evidenced by electrochemical measurements and post-mortem analyses: (1) less nucleation barrier and overpotential, (2) limited zincate formation, (3) improved Zn<sup>2+</sup> flux and (4) efficient Zn plating/stripping, the as-prepared Z8-SA@Cu is rationally considered to be a promising anode for ALZHSCs. Encouragingly, the assembled ALZHSC device not only delivers an impressive rate capability (40 mAh/g at 1 mA/cm<sup>2</sup> and 34 mAh/g at 10 mA/cm<sup>2</sup>) but also achieves the excellent cycling stability (capacity retention: 88 % after 12,000 cycles at 5 mA). Most importantly, the ALZHSC device also reveals significant increases in gravimetric energy density and high-power ability as compared to the traditional ZHSCs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402140"},"PeriodicalIF":7.5,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491611","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Erika Saccullo, Vincenzo Patamia, Chiara Zagni, Antonio Rescifina, Giuseppe Floresta
Nature is a remarkable source of inspiration for developing sustainable and eco-friendly synthetic procedures. In recent years, the synthesis of cyclic carbonates has garnered significant attention due to their versatile applications in various fields, including materials science, pharmaceuticals, and green chemistry. Drawing inspiration from nature, researchers have explored innovative synthetic routes that mimic biological processes to produce cyclic carbonates efficiently and sustainably. This article reviews nature-inspired synthetic procedures for cyclic carbonate formation, highlighting the key strategies and principles employed. Through biomimicry, researchers aim to harness the efficiency and selectivity observed in biological systems to develop greener and more sustainable methods for cyclic carbonate synthesis. Integrating bio-inspired strategies offers opportunities for improving synthetic efficiency and contributes to reducing the environmental impact associated with traditional chemical processes. This review underscores the potential of nature-inspired approaches in advancing the field of cyclic carbonate synthesis toward more sustainable and environmentally benign practices, focusing on recent literature.
{"title":"Learning Strategies from Nature's Blueprint to Cyclic Carbonate Synthesis.","authors":"Erika Saccullo, Vincenzo Patamia, Chiara Zagni, Antonio Rescifina, Giuseppe Floresta","doi":"10.1002/cssc.202402061","DOIUrl":"https://doi.org/10.1002/cssc.202402061","url":null,"abstract":"<p><p>Nature is a remarkable source of inspiration for developing sustainable and eco-friendly synthetic procedures. In recent years, the synthesis of cyclic carbonates has garnered significant attention due to their versatile applications in various fields, including materials science, pharmaceuticals, and green chemistry. Drawing inspiration from nature, researchers have explored innovative synthetic routes that mimic biological processes to produce cyclic carbonates efficiently and sustainably. This article reviews nature-inspired synthetic procedures for cyclic carbonate formation, highlighting the key strategies and principles employed. Through biomimicry, researchers aim to harness the efficiency and selectivity observed in biological systems to develop greener and more sustainable methods for cyclic carbonate synthesis. Integrating bio-inspired strategies offers opportunities for improving synthetic efficiency and contributes to reducing the environmental impact associated with traditional chemical processes. This review underscores the potential of nature-inspired approaches in advancing the field of cyclic carbonate synthesis toward more sustainable and environmentally benign practices, focusing on recent literature.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402061"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491604","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Raphael L Streng, Samuel Reiser, Sabrina Wager, Nykola Pommer, Aliaksandr S Bandarenka
Aqueous alkali-ion batteries are gaining traction as a low-cost, sustainable alternative to conventional organic lithium-ion batteries. However, the rapid degradation of commonly used electrode materials, such as Prussian Blue Analogs and carbonyl-based organic compounds, continues to challenge the economic viability of these devices. While stability issues can be addressed by employing highly concentrated water-in-salt electrolytes, this approach often requires expensive and, in many cases, fluorinated salts. Here, we show that replacing monovalent K+ ions with divalent Ca2+ ions in the electrolyte significantly enhances the stability of both a copper hexacyanoferrate cathode and a polyimide anode. These findings have direct implications for developing an optimized aqueous Ca-ion battery that demonstrates exceptional fast-charging capabilities and ultra-long cycle life and points toward applying Ca-based batteries for large-scale energy storage.
{"title":"A Fast and Highly Stable Aqueous Calcium-Ion Battery for Sustainable Energy Storage.","authors":"Raphael L Streng, Samuel Reiser, Sabrina Wager, Nykola Pommer, Aliaksandr S Bandarenka","doi":"10.1002/cssc.202401469","DOIUrl":"10.1002/cssc.202401469","url":null,"abstract":"<p><p>Aqueous alkali-ion batteries are gaining traction as a low-cost, sustainable alternative to conventional organic lithium-ion batteries. However, the rapid degradation of commonly used electrode materials, such as Prussian Blue Analogs and carbonyl-based organic compounds, continues to challenge the economic viability of these devices. While stability issues can be addressed by employing highly concentrated water-in-salt electrolytes, this approach often requires expensive and, in many cases, fluorinated salts. Here, we show that replacing monovalent K<sup>+</sup> ions with divalent Ca<sup>2+</sup> ions in the electrolyte significantly enhances the stability of both a copper hexacyanoferrate cathode and a polyimide anode. These findings have direct implications for developing an optimized aqueous Ca-ion battery that demonstrates exceptional fast-charging capabilities and ultra-long cycle life and points toward applying Ca-based batteries for large-scale energy storage.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401469"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen peroxide (H2O2) is a versatile and zero-emission material that is widely used in the industrial, domestic, and healthcare sectors. It is clear that it plays a critical role in advancing environmental sustainability, acting as a green energy source, and protecting human health. Conventional production techniques focused on anthraquinone oxidation, however, electrocatalytic synthesis has arisen as a means of utilizing renewable energy sources in conjunction with available resources like oxygen and water. These strides represent a substantial change toward more environmentally and energy-friendly H2O2 manufacturing techniques that are in line with current environmental and energy goals. This work reviews recent advances in two-electron water oxidation reaction (2e-WOR) electrocatalysts, including design principles and reaction mechanisms, examines catalyst design alternatives and experimental characterization techniques, proposes standardized assessment criteria, investigates the impact of the interfacial milieu on the reaction, and discusses the value of in situ characterization and molecular dynamics simulations as a supplement to traditional experimental techniques and theoretical simulations, as shown in Figure 1. The review also emphasizes the importance of device design, interface, and surface engineering in improving the production of H2O2. Through adjustments to the chemical microenvironment, catalysts can demonstrate improved performance, opening the door for commercial applications that are scalable through tandem cell development.
{"title":"Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering.","authors":"Huixuan Cao, Ge Chen, Yong Yan, Dong Wang","doi":"10.1002/cssc.202401100","DOIUrl":"https://doi.org/10.1002/cssc.202401100","url":null,"abstract":"<p><p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a versatile and zero-emission material that is widely used in the industrial, domestic, and healthcare sectors. It is clear that it plays a critical role in advancing environmental sustainability, acting as a green energy source, and protecting human health. Conventional production techniques focused on anthraquinone oxidation, however, electrocatalytic synthesis has arisen as a means of utilizing renewable energy sources in conjunction with available resources like oxygen and water. These strides represent a substantial change toward more environmentally and energy-friendly H<sub>2</sub>O<sub>2</sub> manufacturing techniques that are in line with current environmental and energy goals. This work reviews recent advances in two-electron water oxidation reaction (2e-WOR) electrocatalysts, including design principles and reaction mechanisms, examines catalyst design alternatives and experimental characterization techniques, proposes standardized assessment criteria, investigates the impact of the interfacial milieu on the reaction, and discusses the value of in situ characterization and molecular dynamics simulations as a supplement to traditional experimental techniques and theoretical simulations, as shown in Figure 1. The review also emphasizes the importance of device design, interface, and surface engineering in improving the production of H<sub>2</sub>O<sub>2</sub>. Through adjustments to the chemical microenvironment, catalysts can demonstrate improved performance, opening the door for commercial applications that are scalable through tandem cell development.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401100"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qiuyue Li, Jingjing Liu, Ze Wu, Aomeng Deng, Jiani Liu, Tian Chen, Jianlong Wei, Yiqiong Zhang, Hanwen Liu
Urea, one of the most widely used nitrogen-containing fertilizers globally, is essential for sustainable agriculture. Improving its production is crucial for meeting the increasing demand for fertilizers. Electrocatalytic co-reduction of CO₂ and nitrogenous compounds (NO₂-/NO₃-) has emerged as a promising strategy for green and energy-efficient urea synthesis. However, challenges such as slow reaction kinetics and complex multi-step electron transfers have hindered the development of efficient urea synthesis methods. This review explores recent advances in the electrocatalytic C-N coupling process, focusing on bimetallic catalysts, metal oxide/hydroxide catalysts, and carbon-based catalysts. The review also discusses the future prospects of designing effective catalysts for electrocatalytic C-N coupling to improve urea synthesis.
{"title":"Recent Advances in Electrocatalytic C-N Coupling for Urea Synthesis.","authors":"Qiuyue Li, Jingjing Liu, Ze Wu, Aomeng Deng, Jiani Liu, Tian Chen, Jianlong Wei, Yiqiong Zhang, Hanwen Liu","doi":"10.1002/cssc.202401865","DOIUrl":"10.1002/cssc.202401865","url":null,"abstract":"<p><p>Urea, one of the most widely used nitrogen-containing fertilizers globally, is essential for sustainable agriculture. Improving its production is crucial for meeting the increasing demand for fertilizers. Electrocatalytic co-reduction of CO₂ and nitrogenous compounds (NO₂<sup>-</sup>/NO₃<sup>-</sup>) has emerged as a promising strategy for green and energy-efficient urea synthesis. However, challenges such as slow reaction kinetics and complex multi-step electron transfers have hindered the development of efficient urea synthesis methods. This review explores recent advances in the electrocatalytic C-N coupling process, focusing on bimetallic catalysts, metal oxide/hydroxide catalysts, and carbon-based catalysts. The review also discusses the future prospects of designing effective catalysts for electrocatalytic C-N coupling to improve urea synthesis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401865"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}