Azat F. Akbulatov, Polina G. Novkina, Anastasia A. Bizyaeva, Natalya G. Nikitenko, Victoria V. Ozerova, Nikita A. Slesarenko, Ekaterina A. Khakina, Ekaterina A. Komissarova, Nikita A. Emelianov, Alexander S. Peregudov, Alexander F. Shestakov, Olga A. Kraevaya, Sergey A. Kuklin and Pavel A. Troshin
Fullerene derivative PCBM is a widely used electron transport layer (ETL) in p–i–n structured perovskite solar cells (PSCs). However, the high cost of PCBM, often exceeding that of all other active materials combined (excluding ITO), represents a significant barrier to the large-scale commercialization of PSCs, necessitating the search for more cost-effective alternatives. Herein, nine novel perylenediimide (PDI) dimers are synthesized and employed as ETLs to overcome these challenges. Electrochemical, optoelectronic, and morphological properties of the synthesized compounds were systematically compared with respect to the reference PDI derivative with a thiophene core building block. Correlations were identified between the ability of the developed materials to form high-quality, uniform films and the stabilization of the underlying perovskite layer. A further significant correlation was also observed between the LUMO level of the PDI derivative and the performance of the perovskite devices. These findings offer valuable insights into the targeted design of dimeric perylenediimide derivatives for creating stable and efficient perovskite solar cells.
{"title":"Perylenediimide-based bridged dimers as electron-transport layers in perovskite solar cells with p–i–n configuration","authors":"Azat F. Akbulatov, Polina G. Novkina, Anastasia A. Bizyaeva, Natalya G. Nikitenko, Victoria V. Ozerova, Nikita A. Slesarenko, Ekaterina A. Khakina, Ekaterina A. Komissarova, Nikita A. Emelianov, Alexander S. Peregudov, Alexander F. Shestakov, Olga A. Kraevaya, Sergey A. Kuklin and Pavel A. Troshin","doi":"10.1039/D5SE00716J","DOIUrl":"https://doi.org/10.1039/D5SE00716J","url":null,"abstract":"<p >Fullerene derivative PCBM is a widely used electron transport layer (ETL) in p–i–n structured perovskite solar cells (PSCs). However, the high cost of PCBM, often exceeding that of all other active materials combined (excluding ITO), represents a significant barrier to the large-scale commercialization of PSCs, necessitating the search for more cost-effective alternatives. Herein, nine novel perylenediimide (PDI) dimers are synthesized and employed as ETLs to overcome these challenges. Electrochemical, optoelectronic, and morphological properties of the synthesized compounds were systematically compared with respect to the reference PDI derivative with a thiophene core building block. Correlations were identified between the ability of the developed materials to form high-quality, uniform films and the stabilization of the underlying perovskite layer. A further significant correlation was also observed between the LUMO level of the PDI derivative and the performance of the perovskite devices. These findings offer valuable insights into the targeted design of dimeric perylenediimide derivatives for creating stable and efficient perovskite solar cells.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5894-5903"},"PeriodicalIF":4.1,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145335376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this study, binder-free nickel cobalt oxide (NiCo2O4) nanowire arrays with a cubic spinel structure were directly grown on nickel foam (NF) via an in situ hydrothermal process. The resulting one-dimensional nanowires exhibited a uniform morphology and a favourable bandgap of approximately 1.67 eV, making them ideal candidates as electrode materials for photo-assisted supercapacitors. Electronic structure analysis revealed the coexistence of Ni2+/Ni3+ and Co2+/Co3+ redox pairs, significantly enhancing electrochemical kinetics and facilitating efficient photo-assisted charge storage. Under illumination, the NiCo2O4@NF nanowires demonstrated a remarkable 54% increase in areal capacitance, from 570 to 880 mF cm−2 at 15 mA cm−2, attributed to the efficient separation and storage of photo-generated charges driven by surface polarization effects. An asymmetric supercapacitor device was fabricated with activated carbon (AC) as the anode and NiCo2O4@NF nanowires as the photoactive cathode, maintaining 88% capacitance retention after 1000 illumination cycles. Density functional theory with the on-site Hubbard U correction (DFT + U) calculations further confirmed that nickel substitution in the Co3O4 matrix significantly reduces the bandgap and enhances the magnetic moment, supported by asymmetric spin-resolved density of states and band structure analyses. This research provides valuable insights for developing next-generation photo-assisted energy storage solutions.
在本研究中,采用原位水热法在泡沫镍(NF)上直接生长了具有立方尖晶石结构的无粘结剂镍钴氧化物(NiCo2O4)纳米线阵列。由此得到的一维纳米线具有均匀的形貌和约1.67 eV的良好带隙,使其成为光辅助超级电容器电极材料的理想候选人。电子结构分析表明,Ni2+/Ni3+和Co2+/Co3+氧化还原对共存,显著增强了电化学动力学,促进了高效的光辅助电荷存储。在光照条件下,NiCo2O4@NF纳米线的面电容在15 mA cm - 2下从570到880 mF cm - 2增加了54%,这是由于表面极化效应驱动的光电电荷的有效分离和存储。以活性炭(AC)为阳极,NiCo2O4@NF纳米线为光活性阴极,制备了一种非对称超级电容器器件,在1000次光照循环后保持88%的电容保持率。密度泛函理论和现场Hubbard U校正(DFT + U)计算进一步证实,镍在Co3O4基体中的取代显著减小了带隙,增强了磁矩,这得到了不对称自旋分辨态密度和带结构分析的支持。这项研究为开发下一代光辅助储能解决方案提供了有价值的见解。
{"title":"Unveiling charge dynamics in high-performance binder-free photo-rechargeable supercapacitors","authors":"Aadil Rashid Lone, Sahil Jangra, Maryam Samanian, Aditya Sadhanala and Kavita Pandey","doi":"10.1039/D5SE00700C","DOIUrl":"https://doi.org/10.1039/D5SE00700C","url":null,"abstract":"<p >In this study, binder-free nickel cobalt oxide (NiCo<small><sub>2</sub></small>O<small><sub>4</sub></small>) nanowire arrays with a cubic spinel structure were directly grown on nickel foam (NF) <em>via</em> an <em>in situ</em> hydrothermal process. The resulting one-dimensional nanowires exhibited a uniform morphology and a favourable bandgap of approximately 1.67 eV, making them ideal candidates as electrode materials for photo-assisted supercapacitors. Electronic structure analysis revealed the coexistence of Ni<small><sup>2+</sup></small>/Ni<small><sup>3+</sup></small> and Co<small><sup>2+</sup></small>/Co<small><sup>3+</sup></small> redox pairs, significantly enhancing electrochemical kinetics and facilitating efficient photo-assisted charge storage. Under illumination, the NiCo<small><sub>2</sub></small>O<small><sub>4</sub></small>@NF nanowires demonstrated a remarkable 54% increase in areal capacitance, from 570 to 880 mF cm<small><sup>−2</sup></small> at 15 mA cm<small><sup>−2</sup></small>, attributed to the efficient separation and storage of photo-generated charges driven by surface polarization effects. An asymmetric supercapacitor device was fabricated with activated carbon (AC) as the anode and NiCo<small><sub>2</sub></small>O<small><sub>4</sub></small>@NF nanowires as the photoactive cathode, maintaining 88% capacitance retention after 1000 illumination cycles. Density functional theory with the on-site Hubbard <em>U</em> correction (DFT + <em>U</em>) calculations further confirmed that nickel substitution in the Co<small><sub>3</sub></small>O<small><sub>4</sub></small> matrix significantly reduces the bandgap and enhances the magnetic moment, supported by asymmetric spin-resolved density of states and band structure analyses. This research provides valuable insights for developing next-generation photo-assisted energy storage solutions.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5856-5868"},"PeriodicalIF":4.1,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145335380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Manasa R. Shankar, A. N. Prabhu and Ramakrishna Nayak
Flexible thermoelectric generators (FTEGs) have garnered considerable interest for their potential in energy harvesting applications. This study investigates the synthesis of SnSe and Bi/Te co-doped SnSe polycrystals using the solid-state reaction method, followed by the fabrication of FTEGs using a low-cost, scalable screen-printing technique. Hall effect measurements confirm successful doping, resulting in a transition from p-type to n-type conduction in SnSe. The Seebeck coefficient of the 2% Bi-doped SnSe/SnSe (p–n type) FTEG reaches −1146 μV K−1, enhancing the thermoelectric performance. A maximum power output of 6.8 nW was obtained for a p–n-type FTEG consisting of SnSe and Sn0.98Bi0.02Se0.97Te0.03 at a temperature difference of 120 °C. Thermal conductivity measurements indicate that doping reduces phonon transport due to increased microstrain and dislocation density, which enhance phonon scattering. Furthermore, the FTEGs exhibited excellent mechanical stability, with less than 0.5% change in electrical resistance at bending angles up to 120° and after 500 cycles. These results suggest that Bi/Te co-doped SnSe is a potential candidate for scalable, flexible thermoelectric applications.
{"title":"A co-doping strategy for p- to n-type transition and performance boost in SnSe-based flexible thermoelectric generators","authors":"Manasa R. Shankar, A. N. Prabhu and Ramakrishna Nayak","doi":"10.1039/D5SE00175G","DOIUrl":"https://doi.org/10.1039/D5SE00175G","url":null,"abstract":"<p >Flexible thermoelectric generators (FTEGs) have garnered considerable interest for their potential in energy harvesting applications. This study investigates the synthesis of SnSe and Bi/Te co-doped SnSe polycrystals using the solid-state reaction method, followed by the fabrication of FTEGs using a low-cost, scalable screen-printing technique. Hall effect measurements confirm successful doping, resulting in a transition from p-type to n-type conduction in SnSe. The Seebeck coefficient of the 2% Bi-doped SnSe/SnSe (p–n type) FTEG reaches −1146 μV K<small><sup>−1</sup></small>, enhancing the thermoelectric performance. A maximum power output of 6.8 nW was obtained for a p–n-type FTEG consisting of SnSe and Sn<small><sub>0.98</sub></small>Bi<small><sub>0.02</sub></small>Se<small><sub>0.97</sub></small>Te<small><sub>0.03</sub></small> at a temperature difference of 120 °C. Thermal conductivity measurements indicate that doping reduces phonon transport due to increased microstrain and dislocation density, which enhance phonon scattering. Furthermore, the FTEGs exhibited excellent mechanical stability, with less than 0.5% change in electrical resistance at bending angles up to 120° and after 500 cycles. These results suggest that Bi/Te co-doped SnSe is a potential candidate for scalable, flexible thermoelectric applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5635-5647"},"PeriodicalIF":4.1,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00175g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hannes Liepold, Hendrik Sannemüller, Philipp A. Heizmann, Julian Stiegeler, Tym de Wild, Carolin Klose, Robert Alink, Severin Vierrath, Steven Holdcroft and Andreas Münchinger
In hydrocarbon-based proton exchange membrane fuel cells, cathode catalyst layers (CLs) made from fluorine-free, sulfonated polyphenylenes (e.g., Pemion®) face challenges in balancing sufficient gas transport with low protonic resistance – a tradeoff that is especially pronounced at application-relevant low humidity operation. Here, we address this issue by utilizing unsupported Pt, i.e., platinum black (PtB), as the electrocatalyst to reach very thin CLs (<2.5 μm). When compared to CLs with carbon-supported platinum (Pt/C), evaluation at the same roughness factor (rf) reveals a performance increase from 180 to 420 mA cm−2 at 0.75 V, 50% RH and 95 °C, which is the highest reported performance for a fuel cell with hydrocarbon membrane and CLs and on par with perfluorosulfonic acid reference cells. Accelerated Pt dissolution tests reveal a fast initial rf loss within the first 100 potential cycles for PtB compared to Pt/C (15% vs. 4%), but virtual identical after 30 000 cycles.
在烃基质子交换膜燃料电池中,由无氟磺化聚苯乙烯(例如Pemion®)制成的阴极催化剂层(CLs)在平衡足够的气体传输和低质子阻力方面面临挑战,这在应用相关的低湿度操作中尤其明显。在这里,我们通过使用无支撑Pt,即铂黑(PtB)作为电催化剂来解决这个问题,以达到非常薄的cl (<2.5 μm)。与碳负载铂(Pt/C)燃料电池相比,在相同粗糙度系数(rf)下的评估显示,在0.75 V, 50% RH和95°C下,性能从180 mA cm - 2增加到420 mA cm - 2,这是碳氢化合物膜和CLs燃料电池的最高性能,与全氟磺酸参考电池相当。加速Pt溶解试验显示,与Pt/C相比,PtB在前100个潜在循环内的初始rf损耗很快(15% vs. 4%),但在3万次循环后基本相同。
{"title":"Back to black: utilizing unsupported Pt for thin cathodes in PFSA-free PEM fuel cells","authors":"Hannes Liepold, Hendrik Sannemüller, Philipp A. Heizmann, Julian Stiegeler, Tym de Wild, Carolin Klose, Robert Alink, Severin Vierrath, Steven Holdcroft and Andreas Münchinger","doi":"10.1039/D5SE00809C","DOIUrl":"https://doi.org/10.1039/D5SE00809C","url":null,"abstract":"<p >In hydrocarbon-based proton exchange membrane fuel cells, cathode catalyst layers (CLs) made from fluorine-free, sulfonated polyphenylenes (<em>e.g.</em>, Pemion®) face challenges in balancing sufficient gas transport with low protonic resistance – a tradeoff that is especially pronounced at application-relevant low humidity operation. Here, we address this issue by utilizing unsupported Pt, <em>i.e.</em>, platinum black (PtB), as the electrocatalyst to reach very thin CLs (<2.5 μm). When compared to CLs with carbon-supported platinum (Pt/C), evaluation at the same roughness factor (rf) reveals a performance increase from 180 to 420 mA cm<small><sup>−2</sup></small> at 0.75 V, 50% RH and 95 °C, which is the highest reported performance for a fuel cell with hydrocarbon membrane and CLs and on par with perfluorosulfonic acid reference cells. Accelerated Pt dissolution tests reveal a fast initial rf loss within the first 100 potential cycles for PtB compared to Pt/C (15% <em>vs.</em> 4%), but virtual identical after 30 000 cycles.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5619-5626"},"PeriodicalIF":4.1,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00809c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Aziz Ur Rehman, Christian H. Schwarz, Sina Souzani, Christian Heßke and Marco Haumann
Liquid organic hydrogen carriers (LOHCs) are a promising method for renewable, green hydrogen transportation from the point of generation using renewable energy to the point of demand. Methanol is one such LOHC with advantages such as high hydrogen content, easy transportation and a simple reaction to release the hydrogen. Herein, we reported the use of a novel supported liquid phase (SLP) catalyst in a miniplant to carry out low-temperature methanol steam reforming (MSR) to release hydrogen and subsequently produce electricity using a high-temperature proton exchange membrane fuel cell (HT-PEMFC). This reformed methanol fuel cell (RMFC) setup successfully ran over the course of 45 h experiencing little catalyst deactivation, producing up to 49.2 lN h−1 of hydrogen and up to 39 W electrical power using HT-PEMFC. Comparing between the reformate gas produced using SLP catalyst and pure hydrogen as feed for the fuel cell, the HT-PEMFC showed almost no difference in the voltage–current characteristic curve in the technically relevant operating points between 500 and 700 mV cell voltage. Furthermore, a pinch analysis indicated that the combination of a low-temperature MSR and HT-PEMFC presents an opportunity for heat-integration which could lead to increased efficiency.
{"title":"Methanol-to-electricity via low-temperature steam reforming integrated with a high-temperature PEM fuel cell","authors":"Muhammad Aziz Ur Rehman, Christian H. Schwarz, Sina Souzani, Christian Heßke and Marco Haumann","doi":"10.1039/D5SE00703H","DOIUrl":"https://doi.org/10.1039/D5SE00703H","url":null,"abstract":"<p >Liquid organic hydrogen carriers (LOHCs) are a promising method for renewable, green hydrogen transportation from the point of generation using renewable energy to the point of demand. Methanol is one such LOHC with advantages such as high hydrogen content, easy transportation and a simple reaction to release the hydrogen. Herein, we reported the use of a novel supported liquid phase (SLP) catalyst in a miniplant to carry out low-temperature methanol steam reforming (MSR) to release hydrogen and subsequently produce electricity using a high-temperature proton exchange membrane fuel cell (HT-PEMFC). This reformed methanol fuel cell (RMFC) setup successfully ran over the course of 45 h experiencing little catalyst deactivation, producing up to 49.2 <em>l</em><small><sub>N</sub></small> h<small><sup>−1</sup></small> of hydrogen and up to 39 W electrical power using HT-PEMFC. Comparing between the reformate gas produced using SLP catalyst and pure hydrogen as feed for the fuel cell, the HT-PEMFC showed almost no difference in the voltage–current characteristic curve in the technically relevant operating points between 500 and 700 mV cell voltage. Furthermore, a pinch analysis indicated that the combination of a low-temperature MSR and HT-PEMFC presents an opportunity for heat-integration which could lead to increased efficiency.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5627-5634"},"PeriodicalIF":4.1,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00703h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230136","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Prerna Tripathi, Renna Shakir, Amit Kumar Verma, J. Karthikeyan, Biswajit Ray, A. S. K. Sinha and Shikha Singh
Correction for “Enhanced activity and chlorine protection in prolonged seawater electrolysis using MoS2/sulfonated reduced graphene oxide” by Prerna Tripathi et al., Sustainable Energy Fuels, 2025, 9, 4300–4319, https://doi.org/10.1039/D5SE00541H.
{"title":"Correction: Enhanced activity and chlorine protection in prolonged seawater electrolysis using MoS2/sulfonated reduced graphene oxide","authors":"Prerna Tripathi, Renna Shakir, Amit Kumar Verma, J. Karthikeyan, Biswajit Ray, A. S. K. Sinha and Shikha Singh","doi":"10.1039/D5SE90066B","DOIUrl":"https://doi.org/10.1039/D5SE90066B","url":null,"abstract":"<p >Correction for “Enhanced activity and chlorine protection in prolonged seawater electrolysis using MoS<small><sub>2</sub></small>/sulfonated reduced graphene oxide” by Prerna Tripathi <em>et al.</em>, <em>Sustainable Energy Fuels</em>, 2025, <strong>9</strong>, 4300–4319, https://doi.org/10.1039/D5SE00541H.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5387-5387"},"PeriodicalIF":4.1,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se90066b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121324","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Graziela C. Sedenho, Guilherme H. S. Ghiraldelli, Rodrigo M. Iost, Ricardo Brito-Pereira, Rita Policia, Senentxu Lanceros-Méndez and Frank N. Crespilho
Bioelectrochemical systems (BESs) and engineered living materials (ELMs) are revolutionizing sustainable energy and carbon management by addressing thermodynamic and kinetic barriers in energy conversion and carbon capture. However, misconceptions about the terminology along with a lack of comprehensive environmental footprint and lifecycle assessments still impact the BESs. In this context, this Tutorial Review highlights the distinct roles of bio-batteries and biofuel cells (BFCs) and addresses the substrate-specific effects on electron transfer (ET), carbon flux, and metabolic byproducts. In yeast, the glucose substrate facilitates rapid, high-flux ET suitable for immediate applications, while fructose supports prolonged ET activity, demonstrating flexibility in carbon capture and energy conversion, as the core of the BES. Thermodynamic analysis reveals the energy potential of extracellular polymeric substances (EPSs), storing energy, while kinetic analyses feature the influence of enzymatic efficiency and mass transport limitations. Additionally, ethanol production integrates energy efficiency with environmental sustainability. By overcoming thermodynamic, kinetic, and scalability challenges, BESs and ELMs emerge as transformative tools advancing carbon neutrality, circular economy, and green energy innovation. Strategic research directions, including synthetic biology and scalable materials, are proposed to enhance the modularity and accelerate the transition to commercial viability.
{"title":"Bioelectrochemical systems and engineered living materials: a tutorial on carbon capture and sustainable energy","authors":"Graziela C. Sedenho, Guilherme H. S. Ghiraldelli, Rodrigo M. Iost, Ricardo Brito-Pereira, Rita Policia, Senentxu Lanceros-Méndez and Frank N. Crespilho","doi":"10.1039/D5SE00344J","DOIUrl":"https://doi.org/10.1039/D5SE00344J","url":null,"abstract":"<p >Bioelectrochemical systems (BESs) and engineered living materials (ELMs) are revolutionizing sustainable energy and carbon management by addressing thermodynamic and kinetic barriers in energy conversion and carbon capture. However, misconceptions about the terminology along with a lack of comprehensive environmental footprint and lifecycle assessments still impact the BESs. In this context, this Tutorial Review highlights the distinct roles of bio-batteries and biofuel cells (BFCs) and addresses the substrate-specific effects on electron transfer (ET), carbon flux, and metabolic byproducts. In yeast, the glucose substrate facilitates rapid, high-flux ET suitable for immediate applications, while fructose supports prolonged ET activity, demonstrating flexibility in carbon capture and energy conversion, as the core of the BES. Thermodynamic analysis reveals the energy potential of extracellular polymeric substances (EPSs), storing energy, while kinetic analyses feature the influence of enzymatic efficiency and mass transport limitations. Additionally, ethanol production integrates energy efficiency with environmental sustainability. By overcoming thermodynamic, kinetic, and scalability challenges, BESs and ELMs emerge as transformative tools advancing carbon neutrality, circular economy, and green energy innovation. Strategic research directions, including synthetic biology and scalable materials, are proposed to enhance the modularity and accelerate the transition to commercial viability.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5727-5748"},"PeriodicalIF":4.1,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145335351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Desta M. Ulisso, Pooja K. Bhoj, Sanjay S. Kolekar, Jaeyeong Heo and Anil Vithal Ghule
Designing hierarchically core–shell heterostructured nanocomposite electrode materials with more active sites and delivering enhanced electrochemical performances for supercapacitors is pursued with great interest. With this motivation, herein, we report a facile two-step reflux condensation method for developing heterostructured core–shell nickel manganese layered double hydroxide nanosheets@ZnCo2O4 on a flexible stainless steel mesh substrate (NM-LDH@ZCO/SSM) as a nanocomposite electrode. The ZnCo2O4 nanorods/SSM core structure (ZCO/SSM) facilitates the deposition of the NiMn-LDH shell structure (NM-LDH), forming a core–shell NM-LDH@ZCO/SSM nanocomposite electrode. The structural and morphological characterization studies were done using XRD, FT-IR, FE-SEM, EDAX, XPS, and TEM to confirm the synthesis of the nanocomposite electrode. The NM-LDH@ZCO/SSM nanocomposite demonstrated an ultrahigh specific capacitance of 3169.14 F g−1 at 10 mA cm−2 with a capacitance retention (CR) of 89.3% after 3000 galvanometric charging–discharging (GCD) cycles at a higher current density (CD) of 55 mA cm−2. An asymmetric supercapacitor device fabricated by using the NM-LDH@ZCO/SSM nanocomposite as the cathode and activated carbon (AC/SSM) as the anode exhibited an energy density of 58.7 Wh kg−1 at 2492 W kg−1, and 91% CR after 5000 GCD cycles at 25 mA cm−2. The results reveal that the NM-LDH@ZCO/SSM nanocomposite is one of the potential candidates for high-performance supercapacitors and is expected to pave the way for its future exploration in energy storage devices.
设计具有更多活性位点的分层核壳异质结构纳米复合电极材料,提高超级电容器的电化学性能是人们关注的焦点。基于这一动机,本文报告了一种简单的两步回流冷凝方法,用于在柔性不锈钢网基板(NM-LDH@ZCO/SSM)上制备异质结构核壳镍锰层状双氢氧化物nanosheets@ZnCo2O4作为纳米复合电极。ZnCo2O4纳米棒/SSM核心结构(ZCO/SSM)促进了NiMn-LDH壳结构(NM-LDH)的沉积,形成了核-壳NM-LDH@ZCO/SSM纳米复合电极。采用XRD、FT-IR、FE-SEM、EDAX、XPS、TEM等手段对纳米复合电极的结构和形态进行了表征。NM-LDH@ZCO/SSM纳米复合材料在10 mA cm−2下具有3169.14 F g−1的超高比电容,在55 mA cm−2的高电流密度(CD)下,经过3000次恒流充放电(GCD)循环后,电容保持率(CR)为89.3%。以NM-LDH@ZCO/SSM纳米复合材料为阴极,活性炭(AC/SSM)为阳极制备的非对称超级电容器在2492 W kg - 1下的能量密度为58.7 Wh kg - 1,在25 mA cm - 2下5000 GCD循环后的CR为91%。结果表明,NM-LDH@ZCO/SSM纳米复合材料是高性能超级电容器的潜在候选材料之一,有望为其未来在储能器件中的探索铺平道路。
{"title":"A core–shell heterostructured nickel manganese layered double hydroxide@ZnCo2O4 nanocomposite electrode for enhanced asymmetric supercapacitor applications","authors":"Desta M. Ulisso, Pooja K. Bhoj, Sanjay S. Kolekar, Jaeyeong Heo and Anil Vithal Ghule","doi":"10.1039/D5SE00863H","DOIUrl":"https://doi.org/10.1039/D5SE00863H","url":null,"abstract":"<p >Designing hierarchically core–shell heterostructured nanocomposite electrode materials with more active sites and delivering enhanced electrochemical performances for supercapacitors is pursued with great interest. With this motivation, herein, we report a facile two-step reflux condensation method for developing heterostructured core–shell nickel manganese layered double hydroxide nanosheets@ZnCo<small><sub>2</sub></small>O<small><sub>4</sub></small> on a flexible stainless steel mesh substrate (NM-LDH@ZCO/SSM) as a nanocomposite electrode. The ZnCo<small><sub>2</sub></small>O<small><sub>4</sub></small> nanorods/SSM core structure (ZCO/SSM) facilitates the deposition of the NiMn-LDH shell structure (NM-LDH), forming a core–shell NM-LDH@ZCO/SSM nanocomposite electrode. The structural and morphological characterization studies were done using XRD, FT-IR, FE-SEM, EDAX, XPS, and TEM to confirm the synthesis of the nanocomposite electrode. The NM-LDH@ZCO/SSM nanocomposite demonstrated an ultrahigh specific capacitance of 3169.14 F g<small><sup>−1</sup></small> at 10 mA cm<small><sup>−2</sup></small> with a capacitance retention (CR) of 89.3% after 3000 galvanometric charging–discharging (GCD) cycles at a higher current density (CD) of 55 mA cm<small><sup>−2</sup></small>. An asymmetric supercapacitor device fabricated by using the NM-LDH@ZCO/SSM nanocomposite as the cathode and activated carbon (AC/SSM) as the anode exhibited an energy density of 58.7 Wh kg<small><sup>−1</sup></small> at 2492 W kg<small><sup>−1</sup></small>, and 91% CR after 5000 GCD cycles at 25 mA cm<small><sup>−2</sup></small>. The results reveal that the NM-LDH@ZCO/SSM nanocomposite is one of the potential candidates for high-performance supercapacitors and is expected to pave the way for its future exploration in energy storage devices.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5354-5366"},"PeriodicalIF":4.1,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yashna Khakre, Tyler K. Pham and Smaranda C. Marinescu
With a surge in atmospheric greenhouse gas levels, a switch to carbon-free energy sources, such as hydrogen, is imminent. Herein, the electrocatalytic activity of triphenylenehexathiolate (THT) based coordination polymers (CPs), NiTHT, was studied toward the hydrogen evolution reaction (HER) in acidic medium. Liquid–liquid interfacial synthesis was employed for film synthesis, with a controlled film thickness ranging from 212 nm to 1740 nm. The best performing film exhibited an overpotential of 501 mV vs. RHE to reach a current density of 10 mA cm−2, with a Tafel slope of 98 mV dec−1, indicating that either the Heyrovsky or the Tafel step was rate determining for the catalysis. Additionally, the influence of extrinsic factors (the identity and concentration of the supporting electrolyte and the catalyst loading) and intrinsic factors (thickness and morphology) on the hydrogen evolution activity of the materials was studied and the kinetics of the HER were rationalized. Finally, the long-term stability of the NiTHT films was evaluated and the highest selectivity (faradaic efficiency, FE) for hydrogen evolution was determined to be > 90%. Post-catalysis characterization revealed a retention of structural integrity with ∼12.5% of Ni leaching into the acidic medium employed for the HER. Solvothermally synthesized NiTHT_ST CP showed an improved catalytic overpotential of 301 mV vs. RHE in a pH 1.3 electrolyte solution, with a FE toward the HER of > 90% over 28 h, displaying a more robust phase of the framework compared to that generated via the interfacial method.
{"title":"Tunable electrocatalytic H2 evolution activity of nickel-dithiolene coordination polymers","authors":"Yashna Khakre, Tyler K. Pham and Smaranda C. Marinescu","doi":"10.1039/D5SE01084E","DOIUrl":"https://doi.org/10.1039/D5SE01084E","url":null,"abstract":"<p >With a surge in atmospheric greenhouse gas levels, a switch to carbon-free energy sources, such as hydrogen, is imminent. Herein, the electrocatalytic activity of triphenylenehexathiolate (<strong>THT</strong>) based coordination polymers (CPs), <strong>NiTHT</strong>, was studied toward the hydrogen evolution reaction (HER) in acidic medium. Liquid–liquid interfacial synthesis was employed for film synthesis, with a controlled film thickness ranging from 212 nm to 1740 nm. The best performing film exhibited an overpotential of 501 mV <em>vs.</em> RHE to reach a current density of 10 mA cm<small><sup>−2</sup></small>, with a Tafel slope of 98 mV dec<small><sup>−1</sup></small>, indicating that either the Heyrovsky or the Tafel step was rate determining for the catalysis. Additionally, the influence of extrinsic factors (the identity and concentration of the supporting electrolyte and the catalyst loading) and intrinsic factors (thickness and morphology) on the hydrogen evolution activity of the materials was studied and the kinetics of the HER were rationalized. Finally, the long-term stability of the <strong>NiTHT</strong> films was evaluated and the highest selectivity (faradaic efficiency, FE) for hydrogen evolution was determined to be > 90%. Post-catalysis characterization revealed a retention of structural integrity with ∼12.5% of Ni leaching into the acidic medium employed for the HER. Solvothermally synthesized <strong>NiTHT_ST</strong> CP showed an improved catalytic overpotential of 301 mV <em>vs.</em> RHE in a pH 1.3 electrolyte solution, with a FE toward the HER of > 90% over 28 h, displaying a more robust phase of the framework compared to that generated <em>via</em> the interfacial method.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5869-5881"},"PeriodicalIF":4.1,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145335374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bo zhang, Liguang Qin, Jiaqing Tang, Minghe Zhu, Shiyu Hua, Qinyang Xue, Yunzeng Cui, Shangqi Sun and Chang Guo
Lithium metal is considered the top choice for anode materials due to its exceptionally high energy density (3860 mAh g−1). However, its practical use in lithium metal anodes (LMAs) is limited by significant dendrite growth and an unstable interface between the anode and electrolyte. Herein, 18-crown-6 and fluoroethylene carbonate (FEC) were introduced as combined additives to improve the stability of the electrode/electrolyte interface and enhance long-term cycling performance. The presence of FEC promotes the formation of a LiF-rich solid electrolyte interphase (SEI), which guides lithium deposition and accelerates the transport of Li+ ions. Additionally, 18-crown-6 can eliminate “hotspots” during the lithium deposition and dissolution processes, leading to superior electrochemical performance. By incorporating 1 wt% 18-crown-6 and 10 vol% FEC, Li‖Cu half-cells achieved an impressive average coulombic efficiency of 97%, while Li‖Li symmetric cells demonstrated excellent stability for over 800 hours. When paired with LiFePO4, the Li‖LFP full cell retained approximately 98% of its capacity and maintained a high average coulombic efficiency of 99% after 100 cycles at 0.5C. This research underscores the vital role of 18-crown-6 and FEC in electrolytes, revealing a fresh strategy to reduce lithium dendrite formation in lithium-based energy storage systems.
{"title":"Tailoring the electrolyte/electrode interface with 18-crown-6 and fluoroethylene carbonate for controlled and uniform lithium deposition","authors":"Bo zhang, Liguang Qin, Jiaqing Tang, Minghe Zhu, Shiyu Hua, Qinyang Xue, Yunzeng Cui, Shangqi Sun and Chang Guo","doi":"10.1039/D5SE00848D","DOIUrl":"https://doi.org/10.1039/D5SE00848D","url":null,"abstract":"<p >Lithium metal is considered the top choice for anode materials due to its exceptionally high energy density (3860 mAh g<small><sup>−1</sup></small>). However, its practical use in lithium metal anodes (LMAs) is limited by significant dendrite growth and an unstable interface between the anode and electrolyte. Herein, 18-crown-6 and fluoroethylene carbonate (FEC) were introduced as combined additives to improve the stability of the electrode/electrolyte interface and enhance long-term cycling performance. The presence of FEC promotes the formation of a LiF-rich solid electrolyte interphase (SEI), which guides lithium deposition and accelerates the transport of Li<small><sup>+</sup></small> ions. Additionally, 18-crown-6 can eliminate “hotspots” during the lithium deposition and dissolution processes, leading to superior electrochemical performance. By incorporating 1 wt% 18-crown-6 and 10 vol% FEC, Li‖Cu half-cells achieved an impressive average coulombic efficiency of 97%, while Li‖Li symmetric cells demonstrated excellent stability for over 800 hours. When paired with LiFePO<small><sub>4</sub></small>, the Li‖LFP full cell retained approximately 98% of its capacity and maintained a high average coulombic efficiency of 99% after 100 cycles at 0.5C. This research underscores the vital role of 18-crown-6 and FEC in electrolytes, revealing a fresh strategy to reduce lithium dendrite formation in lithium-based energy storage systems.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5705-5716"},"PeriodicalIF":4.1,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}