Amanuel Gidey Gebretatios, Fawzi Banat and Chin Kui Cheng
To meet the growing global energy demand and keep our planet healthy, more than 10 terawatts of carbon-neutral energy will be required by 2050. H2, which has an energy density of 33.33 kW h kg−1, has been identified as a renewable and clean energy carrier to meet this energy demand and as a substitute for fossil fuels. H2 storage is crucial for harnessing H2 energy to its fullest potential and realizing the H2 economy. Although compression and liquefaction are established H2 storage techniques, safety concerns, energy consumption (up to 18 and 40% of H2's LHV for compression and liquefaction, respectively), and boil-off losses of up to 3% per day in liquefaction remain the main limitations. Researchers currently are exploring safe, compact, and efficient solid-state H2 storage methods. Complex hydrides such as LiBH4, NaBH4, LiAlH4, and NaAlH4, which are formed by the coordination of complex anions such as [BH4]− and [AlH4]− stabilized by metal cations such as Na+, Li+, Mg2+, and Ca2+, are a class of solid-state H2 storage materials with promising storage capacities. In principle, most of them are capable of meeting the ultimate volumetric (0.05 kg H2 per L) and gravimetric (6.5 wt%) storage capacity goals set by the U.S. DoE. However, they suffer from unfavorable thermodynamics-Tdes (150–600 °C), high desorption kinetic barrier-Eades (50–275 kJ mol−1), and limited reversibility. One intriguing approach to address these limitations is nanoconfinement in suitable host materials, benefiting from the synergetic effects of nanosizing, immobilization, destabilization, and, sometimes, catalysis for scaffolds that mutually induce catalytic effects. In this review, major H2 storage techniques are briefly discussed. Developments in the nanoconfinement of complex hydrides, host materials, synthetic methods, characterizations, and advances in improving kinetics, thermodynamics, and reversibility via nanoconfinement are discussed. This paves the way for the use of hydrides in practical H2 economy technologies, and contributes to the advancement of clean energy solutions.
{"title":"A critical review of hydrogen storage: toward the nanoconfinement of complex hydrides from the synthesis and characterization perspectives","authors":"Amanuel Gidey Gebretatios, Fawzi Banat and Chin Kui Cheng","doi":"10.1039/D4SE00353E","DOIUrl":"https://doi.org/10.1039/D4SE00353E","url":null,"abstract":"<p >To meet the growing global energy demand and keep our planet healthy, more than 10 terawatts of carbon-neutral energy will be required by 2050. H<small><sub>2</sub></small>, which has an energy density of 33.33 kW h kg<small><sup>−1</sup></small>, has been identified as a renewable and clean energy carrier to meet this energy demand and as a substitute for fossil fuels. H<small><sub>2</sub></small> storage is crucial for harnessing H<small><sub>2</sub></small> energy to its fullest potential and realizing the H<small><sub>2</sub></small> economy. Although compression and liquefaction are established H<small><sub>2</sub></small> storage techniques, safety concerns, energy consumption (up to 18 and 40% of H<small><sub>2</sub></small>'s LHV for compression and liquefaction, respectively), and boil-off losses of up to 3% per day in liquefaction remain the main limitations. Researchers currently are exploring safe, compact, and efficient solid-state H<small><sub>2</sub></small> storage methods. Complex hydrides such as LiBH<small><sub>4</sub></small>, NaBH<small><sub>4</sub></small>, LiAlH<small><sub>4</sub></small>, and NaAlH<small><sub>4</sub></small>, which are formed by the coordination of complex anions such as [BH<small><sub>4</sub></small>]<small><sup>−</sup></small> and [AlH<small><sub>4</sub></small>]<small><sup>−</sup></small> stabilized by metal cations such as Na<small><sup>+</sup></small>, Li<small><sup>+</sup></small>, Mg<small><sup>2+</sup></small>, and Ca<small><sup>2+</sup></small>, are a class of solid-state H<small><sub>2</sub></small> storage materials with promising storage capacities. In principle, most of them are capable of meeting the ultimate volumetric (0.05 kg H<small><sub>2</sub></small> per L) and gravimetric (6.5 wt%) storage capacity goals set by the U.S. DoE. However, they suffer from unfavorable thermodynamics-<em>T</em><small><sub>des</sub></small> (150–600 °C), high desorption kinetic barrier-<em>E</em><small><sub>ades</sub></small> (50–275 kJ mol<small><sup>−1</sup></small>), and limited reversibility. One intriguing approach to address these limitations is nanoconfinement in suitable host materials, benefiting from the synergetic effects of nanosizing, immobilization, destabilization, and, sometimes, catalysis for scaffolds that mutually induce catalytic effects. In this review, major H<small><sub>2</sub></small> storage techniques are briefly discussed. Developments in the nanoconfinement of complex hydrides, host materials, synthetic methods, characterizations, and advances in improving kinetics, thermodynamics, and reversibility <em>via</em> nanoconfinement are discussed. This paves the way for the use of hydrides in practical H<small><sub>2</sub></small> economy technologies, and contributes to the advancement of clean energy solutions.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 22","pages":" 5091-5130"},"PeriodicalIF":5.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587701","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}
Frank N. Crespilho, Ricardo Brito-Pereira, Rita Policia, Nelson Pereira, Graziela C. Sedenho, Carlos M. Costa and Senentxu Lanceros-Méndez
In this work, we present the development of a fully rechargeable bio-battery, powered by Saccharomyces cerevisiae and utilizing recyclable PET carbon-based electrodes. Through the integration of yeast with the iota-carrageenan hydrogel and potassium ferricyanide as a redox mediator, the bio-battery consistently delivers 450 mV with excellent cyclability. This eco-friendly approach demonstrates great potential for advancing sustainable energy solutions, particularly in powering low-energy applications such as biomedical devices. Ongoing advancements in membrane design are expected to significantly boost the long-term performance and operational stability of this system, further solidifying its applicability in real-world scenarios.
在这项研究中,我们利用可回收的 PET 碳基电极,开发出了一种以酵母菌为动力的完全可充电生物电池。通过将酵母与 iota-carrageenan 水凝胶和作为氧化还原媒介的铁氰化钾相结合,该生物电池可持续提供 450 mV 的电压,并具有出色的循环性。这种生态友好型方法展示了推进可持续能源解决方案的巨大潜力,特别是在为生物医学设备等低能耗应用供电方面。膜设计的不断进步有望显著提高该系统的长期性能和运行稳定性,进一步巩固其在现实世界中的适用性。
{"title":"Yeast bio-batteries†","authors":"Frank N. Crespilho, Ricardo Brito-Pereira, Rita Policia, Nelson Pereira, Graziela C. Sedenho, Carlos M. Costa and Senentxu Lanceros-Méndez","doi":"10.1039/D4SE00903G","DOIUrl":"https://doi.org/10.1039/D4SE00903G","url":null,"abstract":"<p >In this work, we present the development of a fully rechargeable bio-battery, powered by <em>Saccharomyces cerevisiae</em> and utilizing recyclable PET carbon-based electrodes. Through the integration of yeast with the iota-carrageenan hydrogel and potassium ferricyanide as a redox mediator, the bio-battery consistently delivers 450 mV with excellent cyclability. This eco-friendly approach demonstrates great potential for advancing sustainable energy solutions, particularly in powering low-energy applications such as biomedical devices. Ongoing advancements in membrane design are expected to significantly boost the long-term performance and operational stability of this system, further solidifying its applicability in real-world scenarios.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 22","pages":" 5165-5169"},"PeriodicalIF":5.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587704","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}
The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) play a vital role in the functioning of Zn–air batteries and similar energy storage systems. These reactions are kinetically sluggish, which limits the performance of rechargeable Zn–air batteries. An effective bifunctional electrocatalyst that can replace the current noble metal based expensive systems is the need of the hour. In this study, Mn-doped cobalt oxide was synthesized using a cobalt zeolitic imidazolate framework (Co-ZIF) as a template. Mn-doped Co-ZIFs with different Co : Mn ratios (0.5, 1, and 2) were prepared using a single-pot technique and converted into corresponding Mn-doped cobalt oxides via calcination. Structural features were studied using X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Mn-Co3O4 displayed a high Brunauer–Emmett–Teller (BET) surface area of 69 m2 g−1 and a high pore volume. Among all the studied compositions, Mn-Co3O4-1 (Co : Mn = 1) exhibited the best performance, illustrating the crucial role of an optimum level of Mn doping. Mn-Co3O4-1 displayed a low ORR onset potential of 0.94 V and high mass transfer limited current density of 5.65 mA cm−2. The catalyst exhibited a low overpotential of 330 mV at a current density of 10 mA cm−2 for the OER. It also exhibited excellent ORR and OER stability and good bifunctionality, with a potential difference of 0.71 V. This study illustrates the excellent performance of Mn-doped cobalt oxides produced using ZIF templates in oxygen electrocatalysis.
氧还原反应(ORR)和氧进化反应(OER)在锌-空气电池和类似储能系统的运行中起着至关重要的作用。这些反应在动力学上比较迟缓,限制了可充电锌-空气电池的性能。当务之急是找到一种有效的双功能电催化剂,以取代目前基于贵金属的昂贵系统。本研究以钴沸石咪唑酸盐框架(Co-ZIF)为模板合成了掺锰氧化钴。掺锰的 Co-ZIF 具有不同的 Co :采用单锅技术制备了不同钴锰比(0.5、1 和 2)的掺锰 Co-ZIF,并通过煅烧将其转化为相应的掺锰钴氧化物。利用 X 射线衍射、扫描电子显微镜、透射电子显微镜和 X 射线光电子能谱对其结构特征进行了研究。Mn-Co3O4 的布鲁纳-埃美特-泰勒(BET)表面积高达 69 m2 g-1,孔隙率也很高。在所有研究成分中,Mn-Co3O4-1(Co : Mn = 1)表现出最佳性能,说明了最佳掺杂锰水平的关键作用。Mn-Co3O4-1 的 ORR 起始电位较低,为 0.94 V,传质限制电流密度较高,为 5.65 mA cm-2。在 10 mA cm-2 的电流密度下,该催化剂的 OER 过电位较低,仅为 330 mV。这项研究说明了使用 ZIF 模板生产的掺锰钴氧化物在氧电催化中的优异性能。
{"title":"Mn-doped cobalt oxide dodecahedron nanocages as an efficient bifunctional electrocatalyst for zinc–air batteries†","authors":"Sai Vani Terlapu and Ranjit Bauri","doi":"10.1039/D4SE00956H","DOIUrl":"https://doi.org/10.1039/D4SE00956H","url":null,"abstract":"<p >The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) play a vital role in the functioning of Zn–air batteries and similar energy storage systems. These reactions are kinetically sluggish, which limits the performance of rechargeable Zn–air batteries. An effective bifunctional electrocatalyst that can replace the current noble metal based expensive systems is the need of the hour. In this study, Mn-doped cobalt oxide was synthesized using a cobalt zeolitic imidazolate framework (Co-ZIF) as a template. Mn-doped Co-ZIFs with different Co : Mn ratios (0.5, 1, and 2) were prepared using a single-pot technique and converted into corresponding Mn-doped cobalt oxides <em>via</em> calcination. Structural features were studied using X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Mn-Co<small><sub>3</sub></small>O<small><sub>4</sub></small> displayed a high Brunauer–Emmett–Teller (BET) surface area of 69 m<small><sup>2</sup></small> g<small><sup>−1</sup></small> and a high pore volume. Among all the studied compositions, Mn-Co<small><sub>3</sub></small>O<small><sub>4</sub></small>-1 (Co : Mn = 1) exhibited the best performance, illustrating the crucial role of an optimum level of Mn doping. Mn-Co<small><sub>3</sub></small>O<small><sub>4</sub></small>-1 displayed a low ORR onset potential of 0.94 V and high mass transfer limited current density of 5.65 mA cm<small><sup>−2</sup></small>. The catalyst exhibited a low overpotential of 330 mV at a current density of 10 mA cm<small><sup>−2</sup></small> for the OER. It also exhibited excellent ORR and OER stability and good bifunctionality, with a potential difference of 0.71 V. This study illustrates the excellent performance of Mn-doped cobalt oxides produced using ZIF templates in oxygen electrocatalysis.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 22","pages":" 5195-5205"},"PeriodicalIF":5.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587655","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}
Sridivya Chintha, Shahan Atif, Anshuman Chaupatnaik, Alexander Golubnichiy, Artem M. Abakumov and Prabeer Barpanda
Lithium-ion battery technology, currently the most popular form of mobile energy storage, primarily uses graphite as the anode. However, the graphite anode, owing to its low working voltage at high current density, is susceptible to lithium plating and related safety risks. In this direction, perovskite oxides like CaSnO3, more recently PbTiO3, have been explored as alternate anode materials due to their higher operational voltage. Extending this family of perovskites, we introduce a widely used lead-free piezoelectric ceramic Na0.5Bi0.5TiO3 (NBT) as a potential anode for lithium-ion batteries. NBT has an average voltage of 0.7 V and a high capacity of 220 mA h g−1. Ex situ diffraction and spectroscopy tools were used to understand the charge storage mechanism. The oxide undergoes an irreversible conversion reaction in the first discharge, followed by reversible (de)alloying of Bi with Li in the subsequent cycles. This material is airstable, with a capacity retention of 82% up to 50 cycles at a high current of 100 mA g−1 without any optimization. Furthermore, limiting the voltage window increases the cycle life to 200 cycles. Perovskite-type Na0.5Bi0.5TiO3 is proposed as a new Bi-based conversion alloying anode for lithium-ion batteries.
锂离子电池技术是目前最流行的移动能源存储方式,主要使用石墨作为负极。然而,石墨阳极由于在高电流密度下工作电压较低,很容易发生锂镀层和相关的安全风险。在这方面,CaSnO3 和最近的 PbTiO3 等过氧化物氧化物因其较高的工作电压而被探索用作替代负极材料。通过扩展包晶石家族,我们介绍了一种广泛使用的无铅压电陶瓷 Na0.5Bi0.5TiO3(NBT),作为锂离子电池的潜在负极材料。NBT 的平均电压为 0.7 V,容量高达 220 mA h g-1。我们利用原位衍射和光谱工具来了解电荷存储机制。这种氧化物在第一次放电时发生了不可逆的转化反应,随后在随后的循环中发生了锂与铋的可逆(脱)合金化反应。这种材料是可气化的,在 100 mA g-1 的高电流下循环 50 次,容量保持率可达 82%,且无需任何优化。此外,限制电压窗口可将循环寿命延长至 200 次。建议将透辉石型 Na0.5Bi0.5TiO3 作为锂离子电池的新型铋基转换合金负极。
{"title":"Na0.5Bi0.5TiO3 perovskite anode for lithium-ion batteries†","authors":"Sridivya Chintha, Shahan Atif, Anshuman Chaupatnaik, Alexander Golubnichiy, Artem M. Abakumov and Prabeer Barpanda","doi":"10.1039/D4SE00935E","DOIUrl":"https://doi.org/10.1039/D4SE00935E","url":null,"abstract":"<p >Lithium-ion battery technology, currently the most popular form of mobile energy storage, primarily uses graphite as the anode. However, the graphite anode, owing to its low working voltage at high current density, is susceptible to lithium plating and related safety risks. In this direction, perovskite oxides like CaSnO<small><sub>3</sub></small>, more recently PbTiO<small><sub>3</sub></small>, have been explored as alternate anode materials due to their higher operational voltage. Extending this family of perovskites, we introduce a widely used lead-free piezoelectric ceramic Na<small><sub>0.5</sub></small>Bi<small><sub>0.5</sub></small>TiO<small><sub>3</sub></small> (NBT) as a potential anode for lithium-ion batteries. NBT has an average voltage of 0.7 V and a high capacity of 220 mA h g<small><sup>−1</sup></small>. <em>Ex situ</em> diffraction and spectroscopy tools were used to understand the charge storage mechanism. The oxide undergoes an irreversible conversion reaction in the first discharge, followed by reversible (de)alloying of Bi with Li in the subsequent cycles. This material is airstable, with a capacity retention of 82% up to 50 cycles at a high current of 100 mA g<small><sup>−1</sup></small> without any optimization. Furthermore, limiting the voltage window increases the cycle life to 200 cycles. Perovskite-type Na<small><sub>0.5</sub></small>Bi<small><sub>0.5</sub></small>TiO<small><sub>3</sub></small> is proposed as a new Bi-based conversion alloying anode for lithium-ion batteries.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5058-5064"},"PeriodicalIF":5.0,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/se/d4se00935e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452815","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}
Catia Nicoletti, Manuel Orlandi, Luca Dell'Amico and Andrea Sartorel
The synthetic insertion of carbon dioxide into organic scaffolds typically requires the reaction of CO2 with a carbanion (carboxylation step), with the latter being generated through chemical, electrochemical, or photochemical routes. Still, little is known about the energetic and structural requirements of this step. In this work, we unveil the reactivity of CO2 with a selected set of 28 carbanions through DFT calculations and provide linear free-energy relationships that correlate the ΔG0 and the ΔG‡ of the carboxylation step. These reveal a Leffler–Hammond parameter α = 0.26 ± 0.02 and an intrinsic barrier ΔG‡0 = 12.7 ± 0.3 kcal mol−1 (ωb97XD/aug-cc-pvtz//ωb97XD/def2tzvp level of theory), indicative of smooth reactivity of carbanions with CO2. This reactivity is further associated with the basicity of the carbanions (expressed as the pKaH of the conjugate acid), in a linear Brønsted plot between calculated ΔG‡ and experimental pKaH (slope β = 0.40 ± 0.04 kcal mol−1). According to the Mayr–Patz equation, calculations allow the extrapolation of electrophilicity values for CO2 in the range from −15.3 to −18.7, in good agreement with a single reported experimental value of −16.3. Concerning the structural changes occurring in the transition state, the major energy penalty comes from the distortion of CO2. These findings can be useful in designing novel reactivity targeting carbon dioxide fixation.
{"title":"Unveiling the reactivity of CO2 with carbanions: a theoretical analysis of the carboxylation step†","authors":"Catia Nicoletti, Manuel Orlandi, Luca Dell'Amico and Andrea Sartorel","doi":"10.1039/D4SE01065E","DOIUrl":"https://doi.org/10.1039/D4SE01065E","url":null,"abstract":"<p >The synthetic insertion of carbon dioxide into organic scaffolds typically requires the reaction of CO<small><sub>2</sub></small> with a carbanion (carboxylation step), with the latter being generated through chemical, electrochemical, or photochemical routes. Still, little is known about the energetic and structural requirements of this step. In this work, we unveil the reactivity of CO<small><sub>2</sub></small> with a selected set of 28 carbanions through DFT calculations and provide linear free-energy relationships that correlate the Δ<em>G</em><small><sup>0</sup></small> and the Δ<em>G</em><small><sup>‡</sup></small> of the carboxylation step. These reveal a Leffler–Hammond parameter <em>α</em> = 0.26 ± 0.02 and an intrinsic barrier Δ<em>G</em><small><sup>‡</sup></small><small><sub>0</sub></small> = 12.7 ± 0.3 kcal mol<small><sup>−1</sup></small> (ωb97XD/aug-cc-pvtz//ωb97XD/def2tzvp level of theory), indicative of smooth reactivity of carbanions with CO<small><sub>2</sub></small>. This reactivity is further associated with the basicity of the carbanions (expressed as the p<em>K</em><small><sub>aH</sub></small> of the conjugate acid), in a linear Brønsted plot between calculated Δ<em>G</em><small><sup>‡</sup></small> and experimental p<em>K</em><small><sub>aH</sub></small> (slope <em>β</em> = 0.40 ± 0.04 kcal mol<small><sup>−1</sup></small>). According to the Mayr–Patz equation, calculations allow the extrapolation of electrophilicity values for CO<small><sub>2</sub></small> in the range from −15.3 to −18.7, in good agreement with a single reported experimental value of −16.3. Concerning the structural changes occurring in the transition state, the major energy penalty comes from the distortion of CO<small><sub>2</sub></small>. These findings can be useful in designing novel reactivity targeting carbon dioxide fixation.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5050-5057"},"PeriodicalIF":5.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/se/d4se01065e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452814","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}
Mengqing Zhou, Changzhou Chen, Jie Jiang, Yajun Liu and Jianchun Jiang
Exploring lignin depolymerization and modification can yield high-value chemicals and liquid fuels, thereby enhancing resource utilization efficiency and alleviating pressure caused by energy shortages. In this paper, lignin-based carbon materials (Co-ZIF@KL-1 and Co-ZIF@KL-2) loaded with a metal–organic framework (ZIF-67) on kraft lignin biochar (KL) were prepared using two different methods (In situ method and traditional immersion method). In addition, catalysts with Co metal loaded on KL biochar (Co@KL) and ZIF-67 catalyst were also prepared for comparison with the above two different Co-ZIF@KL-1 and Co-ZIF@KL-2 catalysts. These catalysts were all applied to the hydrodeoxygenation (HDO) of guaiacol. Among them, the Co-ZIF@KL-1 catalyst exhibited the highest catalytic activity with 94.53% conversion of guaiacol and 83.86% selectivity of cyclohexanol under the optimal reaction conditions of 240 °C, 2.0 MPa N2, and 4 h. The superior catalytic performance can be attributed to its high surface area, strong stability, and appropriate acidic sites. Based on the distribution of catalytic products, pathways for the guaiacol HDO reaction are hypothesized. In general, ZIF materials and lignin composites offer substantial value for advancing biomass catalytic conversion in the future.
{"title":"Environmentally friendly and innovative design of ZIF-67 and lignin modified composites for efficient catalytic transfer hydrodeoxygenation of lignin-related phenols†","authors":"Mengqing Zhou, Changzhou Chen, Jie Jiang, Yajun Liu and Jianchun Jiang","doi":"10.1039/D4SE01220H","DOIUrl":"https://doi.org/10.1039/D4SE01220H","url":null,"abstract":"<p >Exploring lignin depolymerization and modification can yield high-value chemicals and liquid fuels, thereby enhancing resource utilization efficiency and alleviating pressure caused by energy shortages. In this paper, lignin-based carbon materials (Co-ZIF@KL-1 and Co-ZIF@KL-2) loaded with a metal–organic framework (ZIF-67) on kraft lignin biochar (KL) were prepared using two different methods (<em>In situ</em> method and traditional immersion method). In addition, catalysts with Co metal loaded on KL biochar (Co@KL) and ZIF-67 catalyst were also prepared for comparison with the above two different Co-ZIF@KL-1 and Co-ZIF@KL-2 catalysts. These catalysts were all applied to the hydrodeoxygenation (HDO) of guaiacol. Among them, the Co-ZIF@KL-1 catalyst exhibited the highest catalytic activity with 94.53% conversion of guaiacol and 83.86% selectivity of cyclohexanol under the optimal reaction conditions of 240 °C, 2.0 MPa N<small><sub>2</sub></small>, and 4 h. The superior catalytic performance can be attributed to its high surface area, strong stability, and appropriate acidic sites. Based on the distribution of catalytic products, pathways for the guaiacol HDO reaction are hypothesized. In general, ZIF materials and lignin composites offer substantial value for advancing biomass catalytic conversion in the future.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5001-5012"},"PeriodicalIF":5.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452810","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}
Feifei Li, Junbo Zhang, Yufu Liu, Guanjun Gao, Yi He and Xuzhuang Yang
The catalytic performance of a nickel catalyst in the methanation reaction is strongly influenced by the nickel loading in the catalyst. However, a high nickel content in the catalyst can result in significant nickel agglomeration and sintering, leading to reduction in the number of the active sites available for the methanation reaction, ultimately resulting in poor catalytic performance. Herein, an efficient nickel catalyst with up to 20 wt% of highly dispersed nickel species was successfully synthesized by a straightforward wet chemical method. The optimal composition of the catalyst was selected by using an orthogonal experimental scheme and range analysis method. During the preparation process, acid-treated clay was used as the support, and amino acids were employed as ligands for nickel ions. The amino groups in amino acids can coordinate with the nickel ions, forming nickel-amino acid framework nanocrystals on the clay layers and thus obtaining a catalyst with a high content of highly dispersed nickel species on the clay layers. The catalyst demonstrated an impressive single pass CO conversion of nearly 100% and a methane selectivity exceeding 82% in the CO methanation reaction, and it exhibited a single pass CO2 conversion surpassing 91% and a remarkable 100% methane selectivity in the CO2 methanation process. Furthermore, the catalyst showcased excellent stability throughout both reactions, further highlighting its potential for practical applications. This study offers a promising approach for the synthesis of efficient nickel catalysts with high nickel contents of highly dispersed active sites.
{"title":"A high-loading catalyst of highly dispersed nickel species on acid-treated mesoporous clay layers for efficient CO and CO2 methanation†","authors":"Feifei Li, Junbo Zhang, Yufu Liu, Guanjun Gao, Yi He and Xuzhuang Yang","doi":"10.1039/D4SE01179A","DOIUrl":"https://doi.org/10.1039/D4SE01179A","url":null,"abstract":"<p >The catalytic performance of a nickel catalyst in the methanation reaction is strongly influenced by the nickel loading in the catalyst. However, a high nickel content in the catalyst can result in significant nickel agglomeration and sintering, leading to reduction in the number of the active sites available for the methanation reaction, ultimately resulting in poor catalytic performance. Herein, an efficient nickel catalyst with up to 20 wt% of highly dispersed nickel species was successfully synthesized by a straightforward wet chemical method. The optimal composition of the catalyst was selected by using an orthogonal experimental scheme and range analysis method. During the preparation process, acid-treated clay was used as the support, and amino acids were employed as ligands for nickel ions. The amino groups in amino acids can coordinate with the nickel ions, forming nickel-amino acid framework nanocrystals on the clay layers and thus obtaining a catalyst with a high content of highly dispersed nickel species on the clay layers. The catalyst demonstrated an impressive single pass CO conversion of nearly 100% and a methane selectivity exceeding 82% in the CO methanation reaction, and it exhibited a single pass CO<small><sub>2</sub></small> conversion surpassing 91% and a remarkable 100% methane selectivity in the CO<small><sub>2</sub></small> methanation process. Furthermore, the catalyst showcased excellent stability throughout both reactions, further highlighting its potential for practical applications. This study offers a promising approach for the synthesis of efficient nickel catalysts with high nickel contents of highly dispersed active sites.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 4945-4955"},"PeriodicalIF":5.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452805","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}
Shujing Sha, Mingjian Qin, Xin Yu, Zhibo Xu and Xiaohui Lu
As a clean energy harvesting technology, triboelectric nanogenerators (TENGs) are becoming increasingly crucial in natural energy harvesting. However, due to the characteristics of natural wind, including randomness and broad wind speed ranges, efficient harvesting of wind energy has become a significant obstacle to developing wind energy TENGs. For this purpose, a fast-response triboelectric nanogenerator (FR-TENG). for gust energy capture is proposed in this paper. It contains a multilayer structure with four rotors; the slider mass is different on each layer of the mechanical switch to achieve graded harvesting of wind energy. Experiments proved that by grading settings, the efficiency of harvesting wind energy of the FR-TENG dramatically improves, and the output electrical signal of the FR-TENG can also be significantly enhanced. In the process of charging a 13 μF capacitor at 11.9 m s−1 wind speed, the charging speed of the FR-TENG is approximately 2.25 times that of the Stepless Wind Energy Triboelectric Nanogenerator (S-TENG). When the wind speed is about 9 m s−1, the FR-TENG can light up 640 light-emitting diodes (LEDs) and typically supply power for a thermometer. In addition, after durability testing, the performance of the FRTENG can be maintained at approximately 97%. Therefore, this paper provides a valuable method for collecting efficient and stable wind energy.
{"title":"A fast-response adaptive hierarchical mode triboelectric nanogenerator for random gust energy harvesting†","authors":"Shujing Sha, Mingjian Qin, Xin Yu, Zhibo Xu and Xiaohui Lu","doi":"10.1039/D4SE00869C","DOIUrl":"https://doi.org/10.1039/D4SE00869C","url":null,"abstract":"<p >As a clean energy harvesting technology, triboelectric nanogenerators (TENGs) are becoming increasingly crucial in natural energy harvesting. However, due to the characteristics of natural wind, including randomness and broad wind speed ranges, efficient harvesting of wind energy has become a significant obstacle to developing wind energy TENGs. For this purpose, a fast-response triboelectric nanogenerator (FR-TENG). for gust energy capture is proposed in this paper. It contains a multilayer structure with four rotors; the slider mass is different on each layer of the mechanical switch to achieve graded harvesting of wind energy. Experiments proved that by grading settings, the efficiency of harvesting wind energy of the FR-TENG dramatically improves, and the output electrical signal of the FR-TENG can also be significantly enhanced. In the process of charging a 13 μF capacitor at 11.9 m s<small><sup>−1</sup></small> wind speed, the charging speed of the FR-TENG is approximately 2.25 times that of the Stepless Wind Energy Triboelectric Nanogenerator (S-TENG). When the wind speed is about 9 m s<small><sup>−1</sup></small>, the FR-TENG can light up 640 light-emitting diodes (LEDs) and typically supply power for a thermometer. In addition, after durability testing, the performance of the FRTENG can be maintained at approximately 97%. Therefore, this paper provides a valuable method for collecting efficient and stable wind energy.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 4783-4789"},"PeriodicalIF":5.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397550","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}
Taiyu Cao, Chunliu Zhu, Xinyu Wang, Zhaowei Ji, Huanyu Liang, Jing Shi, Weiqian Tian, Jingwei Chen, Jingyi Wu and Huanlei Wang
Zinc ion hybrid capacitors (ZIHCs) are expected to be one of the most promising energy storage devices due to their affordability, high level of safety, durability and exceptional electrochemical performance. However, the widespread applications of ZIHCs are often hindered by the low specific capacity and energy density of cathode materials. Faced with these challenges, we employed a template strategy to construct oxygen-doped porous carbon nanoflake (PCN) cathode materials with abundant defective sites as a potential candidate for the cathode material of ZIHCs. PCNs possess a substantial specific surface area of 1134 m2 g−1 with a hierarchical porous structure, and a high oxygen doping level of 19.0 at%, offering abundant active sites to enhance the storage capacity of PCN-based ZIHCs. Consequently, ZIHCs assembled from PCNs exhibit an extraordinary specific capacity of 179.3 mA h g−1 at 0.1 A g−1, excellent cycling stability with no obvious capacity decay over 5000 cycles even at 10 A g−1, and an outstanding energy density of 116.7 W h kg−1. Additionally, ex situ experiments were conducted to study the dynamic behaviors (adsorption/desorption) between zinc ions and anions of PCN-based electrodes during the charge and discharge process. This work highlights the importance of introducing rich oxygen-containing functional groups to carbon electrodes for constructing ZIHCs with outstanding performance.
锌离子混合电容器(ZIHC)因其经济实惠、高度安全、经久耐用和优异的电化学性能,有望成为最有前途的储能设备之一。然而,由于阴极材料的比容量和能量密度较低,ZIHC 的广泛应用往往受到阻碍。面对这些挑战,我们采用模板策略构建了具有丰富缺陷位点的氧掺杂多孔碳纳米片(PCN)阴极材料,作为 ZIHC 阴极材料的潜在候选材料。PCN 的比表面积高达 1134 m2 g-1,具有分层多孔结构,氧掺杂水平高达 19.0 at%,可提供丰富的活性位点,从而提高基于 PCN 的 ZIHC 的存储容量。因此,由 PCN 组装而成的 ZIHC 在 0.1 A g-1 的条件下,比容量高达 179.3 mA h g-1;循环稳定性极佳,即使在 10 A g-1 的条件下,5000 次循环也不会出现明显的容量衰减;能量密度高达 116.7 W h kg-1。此外,还进行了原位实验,以研究 PCN 基电极在充放电过程中锌离子与阴离子之间的动态行为(吸附/解吸)。这项研究强调了在碳电极中引入丰富的含氧官能团对于构建性能卓越的 ZIHC 的重要性。
{"title":"Oxygen enriched porous carbon nanoflakes enable high-performance zinc ion hybrid capacitors†","authors":"Taiyu Cao, Chunliu Zhu, Xinyu Wang, Zhaowei Ji, Huanyu Liang, Jing Shi, Weiqian Tian, Jingwei Chen, Jingyi Wu and Huanlei Wang","doi":"10.1039/D4SE00992D","DOIUrl":"https://doi.org/10.1039/D4SE00992D","url":null,"abstract":"<p >Zinc ion hybrid capacitors (ZIHCs) are expected to be one of the most promising energy storage devices due to their affordability, high level of safety, durability and exceptional electrochemical performance. However, the widespread applications of ZIHCs are often hindered by the low specific capacity and energy density of cathode materials. Faced with these challenges, we employed a template strategy to construct oxygen-doped porous carbon nanoflake (PCN) cathode materials with abundant defective sites as a potential candidate for the cathode material of ZIHCs. PCNs possess a substantial specific surface area of 1134 m<small><sup>2</sup></small> g<small><sup>−1</sup></small> with a hierarchical porous structure, and a high oxygen doping level of 19.0 at%, offering abundant active sites to enhance the storage capacity of PCN-based ZIHCs. Consequently, ZIHCs assembled from PCNs exhibit an extraordinary specific capacity of 179.3 mA h g<small><sup>−1</sup></small> at 0.1 A g<small><sup>−1</sup></small>, excellent cycling stability with no obvious capacity decay over 5000 cycles even at 10 A g<small><sup>−1</sup></small>, and an outstanding energy density of 116.7 W h kg<small><sup>−1</sup></small>. Additionally, <em>ex situ</em> experiments were conducted to study the dynamic behaviors (adsorption/desorption) between zinc ions and anions of PCN-based electrodes during the charge and discharge process. This work highlights the importance of introducing rich oxygen-containing functional groups to carbon electrodes for constructing ZIHCs with outstanding performance.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 20","pages":" 4790-4798"},"PeriodicalIF":5.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397551","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}
D. RajaKullayappa, G. Karthikeyan, P. Premkumar, V. Elangkathir and C. G. Saravanan
During the COVID-19 pandemic, disposable masks were widely used, which raised substantial environmental concerns due to their improper disposal and plastic pollution. The masks, primarily made from polypropylene, represent not only an environmental degradation problem, but also an opportunity for energy recovery. In an innovative approach, these used masks were converted into ‘mask oil,’ which can be used as an alternative fuel for diesel engines, providing a sustainable solution to waste management and energy conservation. The mask oil, derived from the degradation of used masks, exhibits properties that make it a viable alternative to conventional diesel fuel. Its low density and kinematic viscosity enable it to atomize and vaporize more rapidly, which results in a greater efficiency of combustion. A lower flash point reduces ignition delay and accelerates combustion initiation, while a higher fire point ensures sustained combustion. According to GC-MS analysis, the mask oil contains a mixture of hydrocarbons and oxygenated compounds that enhance its lubricity and burning properties. FTIR analysis revealed functional groups such as alkenes and alcohols that enhance the reactivity and combustion efficiency of the oil. A test on a Kirloskar TV1 diesel engine demonstrated superior heat release rates and cylinder pressures in comparison to diesel, as well as lower unburned hydrocarbon emissions.
{"title":"Production of mask oil using a biogas-fired reactor with a fly ash catalyst and its assessment in a diesel engine","authors":"D. RajaKullayappa, G. Karthikeyan, P. Premkumar, V. Elangkathir and C. G. Saravanan","doi":"10.1039/D4SE00664J","DOIUrl":"https://doi.org/10.1039/D4SE00664J","url":null,"abstract":"<p >During the COVID-19 pandemic, disposable masks were widely used, which raised substantial environmental concerns due to their improper disposal and plastic pollution. The masks, primarily made from polypropylene, represent not only an environmental degradation problem, but also an opportunity for energy recovery. In an innovative approach, these used masks were converted into ‘mask oil,’ which can be used as an alternative fuel for diesel engines, providing a sustainable solution to waste management and energy conservation. The mask oil, derived from the degradation of used masks, exhibits properties that make it a viable alternative to conventional diesel fuel. Its low density and kinematic viscosity enable it to atomize and vaporize more rapidly, which results in a greater efficiency of combustion. A lower flash point reduces ignition delay and accelerates combustion initiation, while a higher fire point ensures sustained combustion. According to GC-MS analysis, the mask oil contains a mixture of hydrocarbons and oxygenated compounds that enhance its lubricity and burning properties. FTIR analysis revealed functional groups such as alkenes and alcohols that enhance the reactivity and combustion efficiency of the oil. A test on a Kirloskar TV1 diesel engine demonstrated superior heat release rates and cylinder pressures in comparison to diesel, as well as lower unburned hydrocarbon emissions.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 21","pages":" 5013-5030"},"PeriodicalIF":5.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452811","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}