Anam Jalil, Hikmatullah Ahmadi, Fabrice Ndayisenga, Sohail Khan, Atif Ahmad, Xiangyang Wang and Zhisheng Yu
Biohydrogen production from food waste offers a sustainable and carbon-neutral alternative to fossil fuels. However, its large-scale application is limited by the rapid hydrolysis of biodegradable organics, resulting in the accumulation of inhibitory byproducts such as ammonia and volatile fatty acids (VFAs), especially lactic acid. These compounds suppress hydrogen-producing bacteria and reduce system efficiency. Integrating dark fermentation (DF) with microbial electrolysis cells (MECs) has emerged as a promising approach to overcome these limitations by converting residual organics into additional hydrogen via electrohydrogenesis. Optimization of operational parameters such as pH, hydraulic retention time (HRT), and organic loading rate (OLR) further enhances hydrogen yield by minimizing VFA accumulation and improving system stability. Integrated DF–MEC systems have achieved hydrogen yields of up to 1608.6 ± 266.2 mL H2 per g COD consumed and COD removal efficiencies of 78.5 ± 5.7%. Heat pretreatment and the use of genetically engineered microbial strains have been shown to further enhance hydrogen production. Engineered strains have delivered hydrogen yields ranging from 0.47 to 1.88 mol H2 per mol glucose. MEC integration has also demonstrated a 30–40% increase in hydrogen production compared to standalone DF systems. The digestate from lactate-driven DF, enriched with VFAs such as acetate and lactate, provides an excellent substrate for MECs, thereby enhancing electrohydrogenesis. Despite high initial capital costs, the long-term benefits, such as waste valorization, greenhouse gas reduction, and renewable energy recovery, make the DF–MEC system a viable and scalable solution for sustainable hydrogen production from food waste.
从食物垃圾中生产生物氢为化石燃料提供了一种可持续的、碳中和的替代品。然而,它的大规模应用受到生物可降解有机物快速水解的限制,导致氨和挥发性脂肪酸(VFAs),特别是乳酸等抑制副产物的积累。这些化合物抑制产氢细菌,降低系统效率。将暗发酵(DF)与微生物电解细胞(MECs)相结合是克服这些限制的一种很有前途的方法,通过电氢发生将残余有机物转化为额外的氢。通过优化pH、水力停留时间(HRT)和有机负载率(OLR)等操作参数,最大限度地减少VFA积累,提高系统稳定性,进一步提高氢气产量。集成DF-MEC系统的产氢率高达每g COD消耗1608.6±266.2 mL H2, COD去除效率为78.5±5.7%。热预处理和基因工程微生物菌株的使用已被证明可以进一步提高氢气的产量。工程菌株的氢气产量从每摩尔葡萄糖0.47到1.88摩尔氢气不等。MEC集成也表明,与独立的DF系统相比,氢气产量增加了30-40%。乳酸驱动DF的消化液富含乙酸和乳酸等VFAs,为mec提供了良好的底物,从而增强了电氢作用。尽管初始投资成本很高,但其长期效益,如废物增值、温室气体减排和可再生能源回收,使DF-MEC系统成为一种可行的、可扩展的解决方案,用于从食物垃圾中可持续制氢。
{"title":"Integrating dark fermentation and electrohydrogenesis for enhanced biohydrogen production from food waste","authors":"Anam Jalil, Hikmatullah Ahmadi, Fabrice Ndayisenga, Sohail Khan, Atif Ahmad, Xiangyang Wang and Zhisheng Yu","doi":"10.1039/D5SE00571J","DOIUrl":"https://doi.org/10.1039/D5SE00571J","url":null,"abstract":"<p >Biohydrogen production from food waste offers a sustainable and carbon-neutral alternative to fossil fuels. However, its large-scale application is limited by the rapid hydrolysis of biodegradable organics, resulting in the accumulation of inhibitory byproducts such as ammonia and volatile fatty acids (VFAs), especially lactic acid. These compounds suppress hydrogen-producing bacteria and reduce system efficiency. Integrating dark fermentation (DF) with microbial electrolysis cells (MECs) has emerged as a promising approach to overcome these limitations by converting residual organics into additional hydrogen <em>via</em> electrohydrogenesis. Optimization of operational parameters such as pH, hydraulic retention time (HRT), and organic loading rate (OLR) further enhances hydrogen yield by minimizing VFA accumulation and improving system stability. Integrated DF–MEC systems have achieved hydrogen yields of up to 1608.6 ± 266.2 mL H<small><sub>2</sub></small> per g COD consumed and COD removal efficiencies of 78.5 ± 5.7%. Heat pretreatment and the use of genetically engineered microbial strains have been shown to further enhance hydrogen production. Engineered strains have delivered hydrogen yields ranging from 0.47 to 1.88 mol H<small><sub>2</sub></small> per mol glucose. MEC integration has also demonstrated a 30–40% increase in hydrogen production compared to standalone DF systems. The digestate from lactate-driven DF, enriched with VFAs such as acetate and lactate, provides an excellent substrate for MECs, thereby enhancing electrohydrogenesis. Despite high initial capital costs, the long-term benefits, such as waste valorization, greenhouse gas reduction, and renewable energy recovery, make the DF–MEC system a viable and scalable solution for sustainable hydrogen production from food waste.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5432-5457"},"PeriodicalIF":4.1,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00571j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230155","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}
Microbial fuel cells (MFCs) represent a promising green technology for energy recovery from organic waste. In this study, we developed biodegradable composite proton exchange membranes (PEMs) based on poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P3HB4HB) reinforced with reduced graphene oxide (rGO) using a solution casting method. The membranes were systematically characterized and tested in a dual-chamber MFC system. The membrane doped with 7 wt% rGO showed a proton conductivity of 23.3 mS cm−1 at 80 °C, a water uptake of 7.71% and a low oxygen permeability of 2.43 × 10−4 cm s−1. This membrane achieved a power density of 71.3 mW m−2, outperforming the commercial Tion5-W membrane by approximately 50%. The integration of rGO improved thermal, mechanical and electrochemical performance while maintaining the biodegradability of the membrane matrix. These findings highlight the potential of rGO/P3HB4HB membranes as a high-performance and environmentally sustainable alternative to conventional perfluorinated PEMs, especially in decentralized wastewater-to-energy applications.
微生物燃料电池(MFCs)是一种很有前途的从有机废物中回收能源的绿色技术。在这项研究中,我们采用溶液铸造的方法,开发了基于聚(3-羟基丁酸盐-co-4-羟基丁酸盐)(P3HB4HB)的可生物降解复合质子交换膜(PEMs),该膜以还原氧化石墨烯(rGO)增强。在双室MFC系统中对膜进行了系统表征和测试。掺入7 wt% rGO的膜在80℃时的质子电导率为23.3 mS cm - 1,吸水率为7.71%,氧渗透率为2.43 × 10−4 cm s - 1。该膜的功率密度为71.3 mW m−2,比商用的Tion5-W膜高出约50%。还原氧化石墨烯的集成提高了热、机械和电化学性能,同时保持了膜基质的可生物降解性。这些发现突出了氧化石墨烯/P3HB4HB膜作为传统全氟PEMs的高性能和环境可持续替代品的潜力,特别是在分散的废水能源应用中。
{"title":"Biodegradable rGO-reinforced poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P3HB4HB) composite membranes for enhanced power generation in microbial fuel cells: a sustainable alternative to commercial PEMs","authors":"Necla Altin and Ayşe Aytaç","doi":"10.1039/D5SE00980D","DOIUrl":"https://doi.org/10.1039/D5SE00980D","url":null,"abstract":"<p >Microbial fuel cells (MFCs) represent a promising green technology for energy recovery from organic waste. In this study, we developed biodegradable composite proton exchange membranes (PEMs) based on poly(3-hydroxybutyrate-<em>co</em>-4-hydroxybutyrate) (P3HB4HB) reinforced with reduced graphene oxide (rGO) using a solution casting method. The membranes were systematically characterized and tested in a dual-chamber MFC system. The membrane doped with 7 wt% rGO showed a proton conductivity of 23.3 mS cm<small><sup>−1</sup></small> at 80 °C, a water uptake of 7.71% and a low oxygen permeability of 2.43 × 10<small><sup>−4</sup></small> cm s<small><sup>−1</sup></small>. This membrane achieved a power density of 71.3 mW m<small><sup>−2</sup></small>, outperforming the commercial Tion5-W membrane by approximately 50%. The integration of rGO improved thermal, mechanical and electrochemical performance while maintaining the biodegradability of the membrane matrix. These findings highlight the potential of rGO/P3HB4HB membranes as a high-performance and environmentally sustainable alternative to conventional perfluorinated PEMs, especially in decentralized wastewater-to-energy applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5311-5326"},"PeriodicalIF":4.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121316","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}
Mengjuan Xu, Kaige Xu, Yiming Li, Fang Wang, Zhengguo Zhang and Shixiong Min
Heteroatom-doped carbon nanomaterials are commonly employed as electrode materials for supercapacitors (SCs) due to their high accessible surface area, tunable surface chemistry, and unique electronic structures. However, they are generally prepared in fine powdery forms from expensive high-purity metal catalyst and carbon precursors via a tedious synthetic process, limiting their practical application. Herein, we develop a monolithic electrode, denoted as Fe@NCNTs/RB, by directly growing high-density N-doped carbon nanotubes (NCNTs) with encapsulated Fe nanoparticles within a red brick (RB) substrate via the chemical vapor deposition (CVD) method using melamine as the sole C and N sources. During the CVD process, the endogenous Fe species within the RB substrate act as efficient self-generated catalysts for catalyzing the in situ growth of high-density NCNTs from melamine pyrolysis, avoiding the use of external high-purity metal catalysts. The as-fabricated Fe@NCNTs/RB electrode is electrically conductive and mechanically strong and can be directly used as a binder-free electrode for SCs, exhibiting a high areal capacitance (Ca) of 918.75 mF cm−2 at 1.0 mA cm−2 and an excellent rate capability with 34% capacitance retention at 20 mA cm−2. Notably, a symmetric SC assembled with an Fe@NCNTs/RB electrode delivers a high Ca of 277.48 mF cm−2 at 1.0 mA cm−2, an energy density of 11.13 μWh cm−2 at a power density of 269.25 μW cm−2 within a potential window of 0–1.1 V, and excellent cycling stability after 50 000 cycles with 92% capacitance retention and a unit coulombic efficiency at 10 mA cm−2. This work paves a new way for the development of cost-effective and practically applicable monolithic electrodes for high-performance SCs.
杂原子掺杂碳纳米材料由于其高可达表面积、可调表面化学性质和独特的电子结构而被广泛用作超级电容器的电极材料。然而,它们通常是由昂贵的高纯度金属催化剂和碳前体通过繁琐的合成过程以精细粉末形式制备的,限制了它们的实际应用。本文采用化学气相沉积(CVD)方法,以三聚氰胺作为唯一的碳氮源,在红砖(RB)衬底中直接生长高密度掺N碳纳米管(NCNTs),并封装Fe纳米颗粒,开发了一种单片电极Fe@NCNTs/RB。在CVD过程中,RB底物中的内源Fe作为高效的自生催化剂,催化高密度NCNTs在三聚氰胺热解中原位生长,避免了外部高纯度金属催化剂的使用。制备的Fe@NCNTs/RB电极具有导电性和机械强度,可直接用作sc的无粘结剂电极,在1.0 mA cm - 2时具有918.75 mF cm - 2的高面电容(Ca),在20 mA cm - 2时具有34%的电容保持率。值得注意的是,与Fe@NCNTs/RB电极组装的对称SC在1.0 mA cm - 2时具有277.48 mF cm - 2的高Ca,在0-1.1 V的电位窗口内,在269.25 μW cm - 2的功率密度下具有11.13 μWh cm - 2的能量密度,并且在5万次循环后具有优异的循环稳定性,电容保持率为92%,单位库仑效率为10 mA cm - 2。这项工作为开发具有成本效益和实际应用价值的高性能超导单片电极铺平了新的道路。
{"title":"Dense N-doped carbon nanotubes with encapsulated Fe nanoparticles directly grown within red brick as a sustainable monolithic electrode for high-performance supercapacitors","authors":"Mengjuan Xu, Kaige Xu, Yiming Li, Fang Wang, Zhengguo Zhang and Shixiong Min","doi":"10.1039/D5SE01123J","DOIUrl":"https://doi.org/10.1039/D5SE01123J","url":null,"abstract":"<p >Heteroatom-doped carbon nanomaterials are commonly employed as electrode materials for supercapacitors (SCs) due to their high accessible surface area, tunable surface chemistry, and unique electronic structures. However, they are generally prepared in fine powdery forms from expensive high-purity metal catalyst and carbon precursors <em>via</em> a tedious synthetic process, limiting their practical application. Herein, we develop a monolithic electrode, denoted as Fe@NCNTs/RB, by directly growing high-density N-doped carbon nanotubes (NCNTs) with encapsulated Fe nanoparticles within a red brick (RB) substrate <em>via</em> the chemical vapor deposition (CVD) method using melamine as the sole C and N sources. During the CVD process, the endogenous Fe species within the RB substrate act as efficient self-generated catalysts for catalyzing the <em>in situ</em> growth of high-density NCNTs from melamine pyrolysis, avoiding the use of external high-purity metal catalysts. The as-fabricated Fe@NCNTs/RB electrode is electrically conductive and mechanically strong and can be directly used as a binder-free electrode for SCs, exhibiting a high areal capacitance (<em>C</em><small><sub>a</sub></small>) of 918.75 mF cm<small><sup>−2</sup></small> at 1.0 mA cm<small><sup>−2</sup></small> and an excellent rate capability with 34% capacitance retention at 20 mA cm<small><sup>−2</sup></small>. Notably, a symmetric SC assembled with an Fe@NCNTs/RB electrode delivers a high <em>C</em><small><sub>a</sub></small> of 277.48 mF cm<small><sup>−2</sup></small> at 1.0 mA cm<small><sup>−2</sup></small>, an energy density of 11.13 μWh cm<small><sup>−2</sup></small> at a power density of 269.25 μW cm<small><sup>−2</sup></small> within a potential window of 0–1.1 V, and excellent cycling stability after 50 000 cycles with 92% capacitance retention and a unit coulombic efficiency at 10 mA cm<small><sup>−2</sup></small>. This work paves a new way for the development of cost-effective and practically applicable monolithic electrodes for high-performance SCs.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5684-5696"},"PeriodicalIF":4.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230193","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}
Ali Elwalily, Emma Verkama, Franz Mantei, Adiya Kaliyeva, Andrew Pounder, Jörg Sauer and Florian Nestler
Correction for “Sustainable aviation fuel production via the methanol pathway: a technical review” by Ali Elwalily et al., Sustainable Energy Fuels, 2025, https://doi.org/10.1039/D5SE00231A.
{"title":"Correction: Sustainable aviation fuel production via the methanol pathway: a technical review","authors":"Ali Elwalily, Emma Verkama, Franz Mantei, Adiya Kaliyeva, Andrew Pounder, Jörg Sauer and Florian Nestler","doi":"10.1039/D5SE90062J","DOIUrl":"https://doi.org/10.1039/D5SE90062J","url":null,"abstract":"<p >Correction for “Sustainable aviation fuel production <em>via</em> the methanol pathway: a technical review” by Ali Elwalily <em>et al.</em>, <em>Sustainable Energy Fuels</em>, 2025, https://doi.org/10.1039/D5SE00231A.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5386-5386"},"PeriodicalIF":4.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se90062j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121320","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}
Various electrolyte designs have been explored to enhance the temperature dependence of the redox potential (Seebeck coefficient) as it determines the cell voltage of thermo-electrochemical devices such as thermally regenerative electrochemical cycles (TRECs). TRECs require redox couples with both high positive and negative Seebeck coefficients to achieve high performance. In our previous study, ferrocyanide/ferricyanide in a mixture of water and tetrabutylammonium fluoride (TBAF) exhibited a high negative Seebeck coefficient owing to the formation and dissociation of semiclathrate hydrate (SCH) induced by temperature variations. In this study, we found that the formation and dissociation of SCH can also provide a high positive Seebeck coefficient (+16 mV K−1) by increasing the weight ratio of TBAF in the electrolyte. The key factor influencing the increase in the Seebeck coefficient is the change in TBAF concentration in the liquid phase, which significantly affects the redox potential of ferrocyanide/ferricyanide. When the TBAF weight ratio in the electrolyte exceeds that of SCH, the effect of SCH formation on the TBAF concentration in the liquid phase is reversed. Therefore, incorporating SCH can enhance the Seebeck coefficient in both positive and negative directions by tailoring the mixing ratio of TBAF. Additionally, we demonstrated a proof-of-concept TREC using the two electrolytes with high positive and negative Seebeck coefficients. The cell demonstrated a significant temperature dependence of the open-circuit voltage, allowing for a much higher average discharge voltage (271 mV) than charge voltage (145 mV), with a small temperature difference between the charge (299 K) and discharge (294 K) processes.
{"title":"Electrolyte exhibiting a high positive Seebeck coefficient induced by semiclathrate hydrate formation for thermo-electrochemical conversion","authors":"Yohei Matsui and Yuki Maeda","doi":"10.1039/D5SE00924C","DOIUrl":"https://doi.org/10.1039/D5SE00924C","url":null,"abstract":"<p >Various electrolyte designs have been explored to enhance the temperature dependence of the redox potential (Seebeck coefficient) as it determines the cell voltage of thermo-electrochemical devices such as thermally regenerative electrochemical cycles (TRECs). TRECs require redox couples with both high positive and negative Seebeck coefficients to achieve high performance. In our previous study, ferrocyanide/ferricyanide in a mixture of water and tetrabutylammonium fluoride (TBAF) exhibited a high negative Seebeck coefficient owing to the formation and dissociation of semiclathrate hydrate (SCH) induced by temperature variations. In this study, we found that the formation and dissociation of SCH can also provide a high positive Seebeck coefficient (+16 mV K<small><sup>−1</sup></small>) by increasing the weight ratio of TBAF in the electrolyte. The key factor influencing the increase in the Seebeck coefficient is the change in TBAF concentration in the liquid phase, which significantly affects the redox potential of ferrocyanide/ferricyanide. When the TBAF weight ratio in the electrolyte exceeds that of SCH, the effect of SCH formation on the TBAF concentration in the liquid phase is reversed. Therefore, incorporating SCH can enhance the Seebeck coefficient in both positive and negative directions by tailoring the mixing ratio of TBAF. Additionally, we demonstrated a proof-of-concept TREC using the two electrolytes with high positive and negative Seebeck coefficients. The cell demonstrated a significant temperature dependence of the open-circuit voltage, allowing for a much higher average discharge voltage (271 mV) than charge voltage (145 mV), with a small temperature difference between the charge (299 K) and discharge (294 K) processes.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5290-5297"},"PeriodicalIF":4.1,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121314","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}
Nan Wu, Mathieu B. A. Freville, Zhiyi Man, Adérito Fins Carreira, Timothée Derkenne, Corentin Tregouet and Annie Colin
This article is a comment on N. Chapuis and L. Bocquet [Sustainable Energy Fuels, 2025, 9, 2087–2097]. In this work, the authors present an experimental process that shows how it is possible to set up a reverse electrodialysis cell capable of achieving power values of 5 W m−2. This value is the profitability threshold. Our work challenges this claim and questions whether the proposed technique can be scaled up.
本文是对N. Chapuis和L. Bocquet[可持续能源燃料,2025,9,2087-2097]的评论。在这项工作中,作者提出了一个实验过程,展示了如何建立一个能够达到5 W m−2功率值的反向电渗析电池。该值是盈利能力阈值。我们的工作挑战了这一说法,并质疑所提出的技术是否可以扩大规模。
{"title":"Comment on “Boosting large scale capacitive harvesting of osmotic power by dynamic matching of ion exchange kinetics” by N. Chapuis and L. Bocquet, Sustainable Energy Fuels, 2025, 9, 2087","authors":"Nan Wu, Mathieu B. A. Freville, Zhiyi Man, Adérito Fins Carreira, Timothée Derkenne, Corentin Tregouet and Annie Colin","doi":"10.1039/D5SE00381D","DOIUrl":"https://doi.org/10.1039/D5SE00381D","url":null,"abstract":"<p >This article is a comment on N. Chapuis and L. Bocquet [<em>Sustainable Energy Fuels</em>, 2025, 9, 2087–2097]. In this work, the authors present an experimental process that shows how it is possible to set up a reverse electrodialysis cell capable of achieving power values of 5 W m<small><sup>−2</sup></small>. This value is the profitability threshold. Our work challenges this claim and questions whether the proposed technique can be scaled up.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5383-5385"},"PeriodicalIF":4.1,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121322","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}
Kritika Sharma, Shrihari Sankarasubramanian, Zhongyang Wang and Vijay Ramani
This study introduces a direct methanol hydrogen peroxide fuel cell (DMHPFC) using a pH-gradient-enabled microscale bipolar interface (PMBI) to address limitations in direct methanol fuel cells (DMFCs). Unlike conventional fuel cells that use oxygen, the DMHPFC utilizes H2O2, enhancing reactant availability and reaction kinetics. The PMBI maintains separate pH environments at the anode and cathode. The PMBI-DMHPFC combines an alkaline anode for methanol oxidation and an acidic cathode for hydrogen peroxide reduction, achieving a theoretical open-circuit voltage (OCV) of 1.72 V (compared to a theoretical OCV of 1.25 V for DMFCs) and a volumetric energy density of 9.2 kWh l−1 using aqueous methanol (39% vol) and hydrogen peroxide (41% vol). This energy density quadruples that of compressed hydrogen (2.1 kWh l−1 at 69 MPa). This study identifies optimal operating conditions: 5 M methanol with 3 M KOH as anolyte, 5 M hydrogen peroxide with 1.5 M sulfuric acid as catholyte, Nafion 115 (127 μm) as membrane, and flow rate of 2.5 ml min−1 cm−2 – that maximize the power output and minimize activation-, ohmic- and mass transfer losses in DMHPFCs. Performance evaluation reveals a measured OCV of 1.69 V. While the PMBI-DMHPFC surpasses DMFC performance, its high OCV and energy density are not fully translated into high power density due to significantly higher activation and mass transport losses compared to H2–O2 fuel cells, which typically achieve peak power densities above 1000 mW cm−2. The DMHPFC achieves a peak power density of 630 mW cm−2 at the unusually high voltage of 0.8 V, reflecting the unique PMBI design and optimized operating conditions that reduce losses. This steeper voltage drop is attributed to sluggish reaction kinetics, membrane crossover and mass transport limitations. It highlights the potential for improved performance through advanced electrocatalysts, optimized membrane materials and flow design from this promising baseline.
本研究介绍了一种直接甲醇过氧化氢燃料电池(DMHPFC),该电池使用ph梯度微尺度双极界面(PMBI)来解决直接甲醇燃料电池(dmfc)的局限性。与使用氧气的传统燃料电池不同,DMHPFC利用H2O2,提高了反应物的可用性和反应动力学。PMBI在阳极和阴极保持不同的pH环境。PMBI-DMHPFC结合了用于甲醇氧化的碱性阳极和用于过氧化氢还原的酸性阴极,在使用含水甲醇(39% vol)和过氧化氢(41% vol)的情况下,其理论开路电压(OCV)为1.72 V (dmfc的理论OCV为1.25 V),体积能量密度为9.2 kWh l - 1。这种能量密度是压缩氢的四倍(在69 MPa下为2.1 kWh l−1)。本研究确定了最佳操作条件:5 M甲醇和3 M KOH作为阳极电解质,5 M过氧化氢和1.5 M硫酸作为阴极电解质,Nafion 115 (127 μm)作为膜,流速为2.5 ml min - 1 cm - 2,最大限度地提高功率输出,减少dmhpfc的活化、欧姆和传质损失。性能评估显示测量的OCV为1.69 V。虽然PMBI-DMHPFC的性能优于DMFC,但与H2-O2燃料电池相比,它的高OCV和能量密度并不能完全转化为高功率密度,因为它的活化和质量传输损失要高得多,而H2-O2燃料电池的峰值功率密度通常在1000 mW cm - 2以上。DMHPFC在异常高的0.8 V电压下达到630 mW cm−2的峰值功率密度,反映了独特的PMBI设计和优化的工作条件,降低了损耗。这种陡峭的电压降是由于反应动力学缓慢,膜交叉和质量传输的限制。它强调了通过先进的电催化剂、优化的膜材料和流动设计来提高性能的潜力。
{"title":"Enhancing pH-gradient microscale bipolar interfaces (PMBI) enabled direct methanol hydrogen peroxide fuel cell (DMHPFC) performance under varying operating conditions","authors":"Kritika Sharma, Shrihari Sankarasubramanian, Zhongyang Wang and Vijay Ramani","doi":"10.1039/D5SE01042J","DOIUrl":"https://doi.org/10.1039/D5SE01042J","url":null,"abstract":"<p >This study introduces a direct methanol hydrogen peroxide fuel cell (DMHPFC) using a pH-gradient-enabled microscale bipolar interface (PMBI) to address limitations in direct methanol fuel cells (DMFCs). Unlike conventional fuel cells that use oxygen, the DMHPFC utilizes H<small><sub>2</sub></small>O<small><sub>2</sub></small>, enhancing reactant availability and reaction kinetics. The PMBI maintains separate pH environments at the anode and cathode. The PMBI-DMHPFC combines an alkaline anode for methanol oxidation and an acidic cathode for hydrogen peroxide reduction, achieving a theoretical open-circuit voltage (OCV) of 1.72 V (compared to a theoretical OCV of 1.25 V for DMFCs) and a volumetric energy density of 9.2 kWh l<small><sup>−1</sup></small> using aqueous methanol (39% vol) and hydrogen peroxide (41% vol). This energy density quadruples that of compressed hydrogen (2.1 kWh l<small><sup>−1</sup></small> at 69 MPa). This study identifies optimal operating conditions: 5 M methanol with 3 M KOH as anolyte, 5 M hydrogen peroxide with 1.5 M sulfuric acid as catholyte, Nafion 115 (127 μm) as membrane, and flow rate of 2.5 ml min<small><sup>−1</sup></small> cm<small><sup>−2</sup></small> – that maximize the power output and minimize activation-, ohmic- and mass transfer losses in DMHPFCs. Performance evaluation reveals a measured OCV of 1.69 V. While the PMBI-DMHPFC surpasses DMFC performance, its high OCV and energy density are not fully translated into high power density due to significantly higher activation and mass transport losses compared to H<small><sub>2</sub></small>–O<small><sub>2</sub></small> fuel cells, which typically achieve peak power densities above 1000 mW cm<small><sup>−2</sup></small>. The DMHPFC achieves a peak power density of 630 mW cm<small><sup>−2</sup></small> at the unusually high voltage of 0.8 V, reflecting the unique PMBI design and optimized operating conditions that reduce losses. This steeper voltage drop is attributed to sluggish reaction kinetics, membrane crossover and mass transport limitations. It highlights the potential for improved performance through advanced electrocatalysts, optimized membrane materials and flow design from this promising baseline.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 5673-5683"},"PeriodicalIF":4.1,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se01042j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230192","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}
Linxin Lu, Zhuohao Bao, Haotian Zhu, Jingyi Wang, Xiangliang Dang, Yichao Chen, Xianze Yin, Xianjie Wen and Yiheng Song
Transparent radiative cooling materials possess spectrally selective optical characteristics: they exhibit excellent transmissive performance in the visible spectrum range to allow visible light to pass through while demonstrating high emissivity in the atmospheric window. As an inherent property of materials, emissivity is defined as the ratio of radiant power per unit area of a material to that of a blackbody (an ideal radiator) at the same temperature under thermal equilibrium, and it is closely related to thermal radiation. According to Kirchhoff's law, emissivity equals absorptivity under thermal equilibrium conditions. Based on the above characteristics, such materials provide crucial support for sustainable cooling technologies and show broad prospects in the field of green and low-carbon cooling. This paper systematically reviews the principles, material systems, and design strategies of such coolers, focusing on their recent advancements. We comprehensively discuss material selection (hydrogels and thin films), structural design (inorganic materials, photonic crystal multilayers, and metamaterial architectures), performance optimization strategies (enhancing infrared emissivity in the atmospheric window), and their applications in smart windows, energy-efficient buildings, and electronics cooling. Future research should address scalability and durability through cross-scale designs and bio-inspired functionalities, further advancing this field. Ultimately, transparent radiative cooling offers an eco-friendly and energy-efficient solution to meet growing global cooling demands.
{"title":"Application and research progress of transparent radiative cooling materials – a review","authors":"Linxin Lu, Zhuohao Bao, Haotian Zhu, Jingyi Wang, Xiangliang Dang, Yichao Chen, Xianze Yin, Xianjie Wen and Yiheng Song","doi":"10.1039/D5SE00977D","DOIUrl":"https://doi.org/10.1039/D5SE00977D","url":null,"abstract":"<p >Transparent radiative cooling materials possess spectrally selective optical characteristics: they exhibit excellent transmissive performance in the visible spectrum range to allow visible light to pass through while demonstrating high emissivity in the atmospheric window. As an inherent property of materials, emissivity is defined as the ratio of radiant power per unit area of a material to that of a blackbody (an ideal radiator) at the same temperature under thermal equilibrium, and it is closely related to thermal radiation. According to Kirchhoff's law, emissivity equals absorptivity under thermal equilibrium conditions. Based on the above characteristics, such materials provide crucial support for sustainable cooling technologies and show broad prospects in the field of green and low-carbon cooling. This paper systematically reviews the principles, material systems, and design strategies of such coolers, focusing on their recent advancements. We comprehensively discuss material selection (hydrogels and thin films), structural design (inorganic materials, photonic crystal multilayers, and metamaterial architectures), performance optimization strategies (enhancing infrared emissivity in the atmospheric window), and their applications in smart windows, energy-efficient buildings, and electronics cooling. Future research should address scalability and durability through cross-scale designs and bio-inspired functionalities, further advancing this field. Ultimately, transparent radiative cooling offers an eco-friendly and energy-efficient solution to meet growing global cooling demands.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5181-5198"},"PeriodicalIF":4.1,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121359","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}
Syed Muhammad Abbas, Anna Jodlbauer, Martin Wilkening, Helmar Wiltsche, Josef V. Ecker, Christian Ellersdorfer, Gregor Gstrein and Ilie Hanzu
The performance of LIBs deteriorates over time due to various aging mechanisms, among which lithium plating (LP) is critical. This study investigates LP in commercial high-energy graphite-SiOx/NMC pouch LIBs cycled until end-of-life (EOL) under LP-inducing conditions. Employing post-mortem analysis techniques such as 7Li nuclear magnetic resonance (NMR) spectroscopy, inductively coupled plasma optical emission spectroscopy (ICP-OES), and scanning electron microscopy (SEM), we aim to provide a comprehensive understanding of LP. Electrochemical methods such as incremental capacity analysis (ICA) and differential voltage analysis (DVA) were first used to identify LP occurrence in a cell during artificial ageing (AA). Subsequently, the cells were dissected to prepare post-mortem analysis samples. ICP-OES revealed an increased soluble lithium (Li) content on the anode surface compared to a fresh cell, which is attributed to LP. Metallic Li was identified on the anode surface of the cycled cell by 7Li NMR at Knight shifts in the range from 245 to 270 ppm, whereas no metallic Li was detected in fresh cell. Post-mortem SEM analysis revealed a mossy layer growth on anode sample of the artificially aged cells that is absent on the anode surface of a fresh cell. This mossy growth is attributed to LP. Elemental mapping also revealed fluorine hotspots on the mossy metallic Li layer, indicating the formation of lithium fluoride (LiF) as a reaction product between metallic Li and the cell electrolyte. Additionally, as the SEM sample was exposed to air during transfer, oxygen hotspot on mossy Li layer in elemental mapping indicates the reaction of oxygen and moisture with metallic Li.
{"title":"Post-mortem identification of lithium plating in high energy automotive batteries","authors":"Syed Muhammad Abbas, Anna Jodlbauer, Martin Wilkening, Helmar Wiltsche, Josef V. Ecker, Christian Ellersdorfer, Gregor Gstrein and Ilie Hanzu","doi":"10.1039/D5SE00509D","DOIUrl":"https://doi.org/10.1039/D5SE00509D","url":null,"abstract":"<p >The performance of LIBs deteriorates over time due to various aging mechanisms, among which lithium plating (LP) is critical. This study investigates LP in commercial high-energy graphite-SiO<small><sub><em>x</em></sub></small>/NMC pouch LIBs cycled until end-of-life (EOL) under LP-inducing conditions. Employing post-mortem analysis techniques such as <small><sup>7</sup></small>Li nuclear magnetic resonance (NMR) spectroscopy, inductively coupled plasma optical emission spectroscopy (ICP-OES), and scanning electron microscopy (SEM), we aim to provide a comprehensive understanding of LP. Electrochemical methods such as incremental capacity analysis (ICA) and differential voltage analysis (DVA) were first used to identify LP occurrence in a cell during artificial ageing (AA). Subsequently, the cells were dissected to prepare post-mortem analysis samples. ICP-OES revealed an increased soluble lithium (Li) content on the anode surface compared to a fresh cell, which is attributed to LP. Metallic Li was identified on the anode surface of the cycled cell by <small><sup>7</sup></small>Li NMR at Knight shifts in the range from 245 to 270 ppm, whereas no metallic Li was detected in fresh cell. Post-mortem SEM analysis revealed a mossy layer growth on anode sample of the artificially aged cells that is absent on the anode surface of a fresh cell. This mossy growth is attributed to LP. Elemental mapping also revealed fluorine hotspots on the mossy metallic Li layer, indicating the formation of lithium fluoride (LiF) as a reaction product between metallic Li and the cell electrolyte. Additionally, as the SEM sample was exposed to air during transfer, oxygen hotspot on mossy Li layer in elemental mapping indicates the reaction of oxygen and moisture with metallic Li.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5342-5353"},"PeriodicalIF":4.1,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00509d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121318","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}
Lipika Sarkar, Sunanda Pal, Sutanu Das, Farhin Sultana, Arnab Banerjee, Bibhutibhushan Show and Upendranath Nandi
An eco-friendly and cost-effective reflux approach is employed to synthesize ZnO-doped NiCo2O4 (NCOXZnO) nanocomposites for supercapacitor applications. Advanced sophisticated tools are employed to investigate the structure, surface morphology, magnetic properties, surface area, and optical characteristics of NCOXZnO nanocomposites to validate their purity. The findings revealed that doping of ZnO significantly influenced the particle size, paramagnetic behaviour, porosity, and active surface area of the pristine NCO material. Electrochemical studies show that NCO7ZnO with 7 wt% ZnO achieves optimal performance, with a specific capacitance of 293 F g−1 at a specific current of 0.5 A g−1 and 439 F g−1 at a scan rate of 1 mV s−1 in 0.5 M H2SO4, surpassing pristine NCO. The NCO7ZnO nanocomposite also shows a high surface area (100.755 m2 g−1), higher pore volume (0.148 cm3 g−1), and low charge transfer resistance (Rct = 0.68 Ω). Additionally, the symmetric supercapacitor device using NCO7ZnO has a superior specific energy of 34.35 W h kg−1 at a specific power of 200 W kg−1. Furthermore, it demonstrates an impressive cycle stability of 98% over 10 000 cycles, positioning ZnO-doped NiCo2O4 as a highly promising candidate for next-generation supercapacitors.
采用一种环保、经济的回流方法合成了用于超级电容器的zno掺杂NiCo2O4 (NCOXZnO)纳米复合材料。采用先进的精密工具研究了NCOXZnO纳米复合材料的结构、表面形貌、磁性能、表面积和光学特性,以验证其纯度。结果表明,ZnO的掺杂显著影响了原始NCO材料的粒径、顺磁性、孔隙率和活性表面积。电化学研究表明,ZnO质量分数为7 wt%的NCO7ZnO具有最佳性能,在0.5 a g−1比电流下比电容为293 F g−1,在0.5 M H2SO4中扫描速率为1 mV s−1时比电容为439 F g−1,优于原始NCO。NCO7ZnO纳米复合材料具有较高的比表面积(100.755 m2 g−1)、较高的孔体积(0.148 cm3 g−1)和较低的电荷转移阻力(Rct = 0.68 Ω)。此外,使用NCO7ZnO的对称超级电容器器件在200 W kg−1的比功率下具有34.35 W h kg−1的优越比能量。此外,它在10,000次循环中表现出98%的令人印象深刻的循环稳定性,将zno掺杂的NiCo2O4定位为下一代超级电容器的非常有前途的候选者。
{"title":"Enhanced cycling stability of ZnO-doped NiCo2O4 electrodes for acidic solid-state symmetric supercapacitors","authors":"Lipika Sarkar, Sunanda Pal, Sutanu Das, Farhin Sultana, Arnab Banerjee, Bibhutibhushan Show and Upendranath Nandi","doi":"10.1039/D5SE00707K","DOIUrl":"https://doi.org/10.1039/D5SE00707K","url":null,"abstract":"<p >An eco-friendly and cost-effective reflux approach is employed to synthesize ZnO-doped NiCo<small><sub>2</sub></small>O<small><sub>4</sub></small> (NCOXZnO) nanocomposites for supercapacitor applications. Advanced sophisticated tools are employed to investigate the structure, surface morphology, magnetic properties, surface area, and optical characteristics of NCOXZnO nanocomposites to validate their purity. The findings revealed that doping of ZnO significantly influenced the particle size, paramagnetic behaviour, porosity, and active surface area of the pristine NCO material. Electrochemical studies show that NCO7ZnO with 7 wt% ZnO achieves optimal performance, with a specific capacitance of 293 F g<small><sup>−1</sup></small> at a specific current of 0.5 A g<small><sup>−1</sup></small> and 439 F g<small><sup>−1</sup></small> at a scan rate of 1 mV s<small><sup>−1</sup></small> in 0.5 M H<small><sub>2</sub></small>SO<small><sub>4</sub></small>, surpassing pristine NCO. The NCO7ZnO nanocomposite also shows a high surface area (100.755 m<small><sup>2</sup></small> g<small><sup>−1</sup></small>), higher pore volume (0.148 cm<small><sup>3</sup></small> g<small><sup>−1</sup></small>), and low charge transfer resistance (<em>R</em><small><sub>ct</sub></small> = 0.68 Ω). Additionally, the symmetric supercapacitor device using NCO7ZnO has a superior specific energy of 34.35 W h kg<small><sup>−1</sup></small> at a specific power of 200 W kg<small><sup>−1</sup></small>. Furthermore, it demonstrates an impressive cycle stability of 98% over 10 000 cycles, positioning ZnO-doped NiCo<small><sub>2</sub></small>O<small><sub>4</sub></small> as a highly promising candidate for next-generation supercapacitors.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 19","pages":" 5327-5341"},"PeriodicalIF":4.1,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145121317","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}