Carles Tortosa, Marina Navarro-Segarra, Pedro Guerrero, Koro de la Caba and Juan Pablo Esquivel
Environmental impacts from the fashion industry are at the top of global pollution. Fiber production, fabric preparation and distribution, and disposal of textiles combined with the excessive consumerism of clothing result in the wastage of thousands of million cubic meters of fresh water, the release of gigatons of CO2 equivalent, and tens of millions of metric tons of textile waste generation every year. This situation shows that there is an urgent and mandatory need to change the fashion paradigm, but, even if accomplished, the current textile waste spread worldwide still needs to be managed in an environmentally conscious way. Upcycling textile waste by pyrolysis is gaining interest as an alternative management option. The goal is to endow waste with new functionalities for its repurposing into new applications. This study focuses on applying pyrolysis to convert discarded clothing into a conductive carbon textile while avoiding treatments with hazardous chemicals. Envisioned to be applied for current collection in all-organic primary power sources, the ultimate goal is to replace synthetic polymers in commercial carbon current collectors. Actual textile waste has been successfully pyrolyzed without the need for pre-treatments or activation. The structural composition of the samples was studied by SEM, X-ray diffraction, Raman spectroscopy, ATR-FTIR spectroscopy, EDS and BET surface area. Electrical and electrochemical characterization showed their suitability as current collectors, which was demonstrated by building an aqueous metal-free organic primary battery. A system of innocuous quinone-based redox chemistry coupled with the revalorized collectors delivered 11.17 mA cm−2 and 1.4 mW cm−2 of power density, proving the feasibility of the proposed application.
{"title":"Conductive carbon fabric generation from single-step upcycling of textile waste†","authors":"Carles Tortosa, Marina Navarro-Segarra, Pedro Guerrero, Koro de la Caba and Juan Pablo Esquivel","doi":"10.1039/D3SE01722B","DOIUrl":"10.1039/D3SE01722B","url":null,"abstract":"<p >Environmental impacts from the fashion industry are at the top of global pollution. Fiber production, fabric preparation and distribution, and disposal of textiles combined with the excessive consumerism of clothing result in the wastage of thousands of million cubic meters of fresh water, the release of gigatons of CO<small><sub>2</sub></small> equivalent, and tens of millions of metric tons of textile waste generation every year. This situation shows that there is an urgent and mandatory need to change the fashion paradigm, but, even if accomplished, the current textile waste spread worldwide still needs to be managed in an environmentally conscious way. Upcycling textile waste by pyrolysis is gaining interest as an alternative management option. The goal is to endow waste with new functionalities for its repurposing into new applications. This study focuses on applying pyrolysis to convert discarded clothing into a conductive carbon textile while avoiding treatments with hazardous chemicals. Envisioned to be applied for current collection in all-organic primary power sources, the ultimate goal is to replace synthetic polymers in commercial carbon current collectors. Actual textile waste has been successfully pyrolyzed without the need for pre-treatments or activation. The structural composition of the samples was studied by SEM, X-ray diffraction, Raman spectroscopy, ATR-FTIR spectroscopy, EDS and BET surface area. Electrical and electrochemical characterization showed their suitability as current collectors, which was demonstrated by building an aqueous metal-free organic primary battery. A system of innocuous quinone-based redox chemistry coupled with the revalorized collectors delivered 11.17 mA cm<small><sup>−2</sup></small> and 1.4 mW cm<small><sup>−2</sup></small> of power density, proving the feasibility of the proposed application.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528108","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}
Prakash Prashanth, Jad Elmourad, Carla Grobler, Stewart Isaacs, Syed Shayan Zahid, James Abel, Christoph Falter, Thibaud Fritz, Florian Allroggen, Jayant S. Sabnis, Sebastian D. Eastham, Raymond L. Speth, Steven R. H. Barrett
The fundamental challenge facing today's aviation industry is to achieve net zero climate impacts while simultaneously sustaining growth and global connectivity. Aviation's impact on surface air quality, which is comparable to aviation's climate impact when monetized, further heightens this challenge. Prior studies have proposed solutions that aim to mitigate either aviation's climate or air quality impacts. No previous work has proposed an aircraft-energy system that simultaneously addresses both aviation's climate and air quality impacts. In this paper we (1) use a multi-disciplinary design approach to optimize aircraft and propulsion systems, (2) estimate lifecycle costs and emissions of producing sustainable fuels including the embodied emissions associated with electricity generation and fuel production, (3) use trajectory optimization to quantify the fuel penalty to avoid persistent contrail formation based on a full year of global flight operations (including, for the first time, contrail avoidance for a hydrogen burning aircraft), and (4) quantify climate and air quality benefits of the proposed solutions using a simplified climate model and sensitivities derived from a global chemistry transport model. We propagate uncertainties in environmental impacts using a Monte-Carlo approach. We use these models to propose and analyze near-zero environmental impact aircraft, which we define as having net zero climate warming and a greater than 95% reduction in air quality impacts relative to present day. We contrast the environmental impacts of today's aircraft-energy system against one built around either “drop-in” fuels or hydrogen. We find that a “zero-impact” aircraft is possible using either hydrogen or power-to-liquid “drop-in” fuels. The proposed aircraft-energy systems reduce combined climate and air quality impacts by 99%, with fuel costs increasing by 40% for hydrogen and 70% for power-to-liquid fueled aircraft relative to today's fleet (i.e., within the range of historical jet fuel price variation). Beyond the specific case presented here, this work presents a framework for holistic analysis of future aviation systems that considers both climate and air quality impacts.
{"title":"Near-zero environmental impact aircraft","authors":"Prakash Prashanth, Jad Elmourad, Carla Grobler, Stewart Isaacs, Syed Shayan Zahid, James Abel, Christoph Falter, Thibaud Fritz, Florian Allroggen, Jayant S. Sabnis, Sebastian D. Eastham, Raymond L. Speth, Steven R. H. Barrett","doi":"10.1039/d4se00419a","DOIUrl":"https://doi.org/10.1039/d4se00419a","url":null,"abstract":"The fundamental challenge facing today's aviation industry is to achieve net zero climate impacts while simultaneously sustaining growth and global connectivity. Aviation's impact on surface air quality, which is comparable to aviation's climate impact when monetized, further heightens this challenge. Prior studies have proposed solutions that aim to mitigate either aviation's climate or air quality impacts. No previous work has proposed an aircraft-energy system that simultaneously addresses both aviation's climate and air quality impacts. In this paper we (1) use a multi-disciplinary design approach to optimize aircraft and propulsion systems, (2) estimate lifecycle costs and emissions of producing sustainable fuels including the embodied emissions associated with electricity generation and fuel production, (3) use trajectory optimization to quantify the fuel penalty to avoid persistent contrail formation based on a full year of global flight operations (including, for the first time, contrail avoidance for a hydrogen burning aircraft), and (4) quantify climate and air quality benefits of the proposed solutions using a simplified climate model and sensitivities derived from a global chemistry transport model. We propagate uncertainties in environmental impacts using a Monte-Carlo approach. We use these models to propose and analyze near-zero environmental impact aircraft, which we define as having net zero climate warming and a greater than 95% reduction in air quality impacts relative to present day. We contrast the environmental impacts of today's aircraft-energy system against one built around either “drop-in” fuels or hydrogen. We find that a “zero-impact” aircraft is possible using either hydrogen or power-to-liquid “drop-in” fuels. The proposed aircraft-energy systems reduce combined climate and air quality impacts by 99%, with fuel costs increasing by 40% for hydrogen and 70% for power-to-liquid fueled aircraft relative to today's fleet (<em>i.e.</em>, within the range of historical jet fuel price variation). Beyond the specific case presented here, this work presents a framework for holistic analysis of future aviation systems that considers both climate and air quality impacts.","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528020","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}
Ilya V. Martynov, Aleksandra N. Zhivchikova, Mikhail D. Tereshchenko, Ilya E. Kuznetsov, Stepan Baryshev, Valentyn S. Volkov, Marina Tepliakova, Alexander V. Akkuratov and Aleksey V. Arsenin
There is a renascence in the use of triphenylamine (TPA)-based donor materials in the field of perovskite photovoltaics. This work presents the synthesis of two novel conjugated small molecules (CSMs), TPA-t and TPA-t EH, which are functionalized with triisopropylsilyl groups and 2-ethylhexyl side chains. These molecules show promise as hole transport materials, which possess high hole mobilities of 1.5 × 10−4 and 2.9 × 10−3 cm2 V−1 s−1. TPA-t and TPA-t EH possess HOMO energy levels at −5.38 and −5.31 eV, which are well-aligned with the valence band of standard perovskite MAPbI3. This resulted in outstanding open-circuit voltages of 1100 and 1080 mV. TPA-based molecules were investigated as HTLs in n-i-p PSCs without additional doping and enabled high efficiency (17.3%) same as for devices with the state-of-the-art polytriarylamine (PTAA) HTL. The obtained results suggest that the developed materials could potentially compete with PTAA with further material structure modification.
{"title":"Conjugated small molecules based on alkylsilyl-modified triphenylamine: promising hole transport materials in perovskite photovoltaics†","authors":"Ilya V. Martynov, Aleksandra N. Zhivchikova, Mikhail D. Tereshchenko, Ilya E. Kuznetsov, Stepan Baryshev, Valentyn S. Volkov, Marina Tepliakova, Alexander V. Akkuratov and Aleksey V. Arsenin","doi":"10.1039/D4SE00521J","DOIUrl":"10.1039/D4SE00521J","url":null,"abstract":"<p >There is a renascence in the use of triphenylamine (TPA)-based donor materials in the field of perovskite photovoltaics. This work presents the synthesis of two novel conjugated small molecules (CSMs), <strong>TPA-t</strong> and <strong>TPA-t EH</strong>, which are functionalized with triisopropylsilyl groups and 2-ethylhexyl side chains. These molecules show promise as hole transport materials, which possess high hole mobilities of 1.5 × 10<small><sup>−4</sup></small> and 2.9 × 10<small><sup>−3</sup></small> cm<small><sup>2</sup></small> V<small><sup>−1</sup></small> s<small><sup>−1</sup></small>. <strong>TPA-t</strong> and <strong>TPA-t EH</strong> possess HOMO energy levels at −5.38 and −5.31 eV, which are well-aligned with the valence band of standard perovskite MAPbI<small><sub>3</sub></small>. This resulted in outstanding open-circuit voltages of 1100 and 1080 mV. TPA-based molecules were investigated as HTLs in n-i-p PSCs without additional doping and enabled high efficiency (17.3%) same as for devices with the state-of-the-art polytriarylamine (PTAA) HTL. The obtained results suggest that the developed materials could potentially compete with PTAA with further material structure modification.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528021","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}
Narendra Naik Deshavath, William Woodruff and Vijay Singh
Hydrothermal pretreatment is a promising approach to lignocellulosic biomass processing for enzymatic hydrolysis and high-yield bioethanol fermentation, as it reduces downstream inhibitor content and the amount of toxic byproducts generated. In this study, the ethanol yield and productivity of an engineered xylose-fermenting strain of Saccharomyces cerevisiae were tested on lignocellulosic hydrolysates produced with varying citrate buffer concentration, solid loading, supplemental nitrogen source, and feedstock of origin, and a semi-integrated bioprocess which integrates enzymatic hydrolysis and bioethanol fermentation was developed. The greatest ethanol yields (gp/gs) of 0.490 ± 0.008, 0.460 ± 0.001, 0.420 ± 0.002 and 0.410 ± 0.002 were obtained from bioenergy sorghum (BES), Miscanthus × giganteus (MG), energy cane (EC), and oilcane (OC), respectively. In addition, an equivalent of 291 L, 253.54 L, 257.8 L, and 260.3 L of bioethanol were produced per ton of BES, MG, EC, and OC, respectively, by using urea as a nitrogen source in a bioreactor.
{"title":"Sustainable strategies to achieve industrial ethanol titers from different bioenergy feedstocks: scale-up approach for better ethanol yield†","authors":"Narendra Naik Deshavath, William Woodruff and Vijay Singh","doi":"10.1039/D4SE00520A","DOIUrl":"10.1039/D4SE00520A","url":null,"abstract":"<p >Hydrothermal pretreatment is a promising approach to lignocellulosic biomass processing for enzymatic hydrolysis and high-yield bioethanol fermentation, as it reduces downstream inhibitor content and the amount of toxic byproducts generated. In this study, the ethanol yield and productivity of an engineered xylose-fermenting strain of <em>Saccharomyces cerevisiae</em> were tested on lignocellulosic hydrolysates produced with varying citrate buffer concentration, solid loading, supplemental nitrogen source, and feedstock of origin, and a semi-integrated bioprocess which integrates enzymatic hydrolysis and bioethanol fermentation was developed. The greatest ethanol yields (g<small><sub>p</sub></small>/g<small><sub>s</sub></small>) of 0.490 ± 0.008, 0.460 ± 0.001, 0.420 ± 0.002 and 0.410 ± 0.002 were obtained from bioenergy sorghum (BES), <em>Miscanthus</em> × <em>giganteus</em> (MG), energy cane (EC), and oilcane (OC), respectively. In addition, an equivalent of 291 L, 253.54 L, 257.8 L, and 260.3 L of bioethanol were produced per ton of BES, MG, EC, and OC, respectively, by using urea as a nitrogen source in a bioreactor.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141506647","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}
Sb2Se3 is a promising photocathode with good stability and large theoretical photocurrent density but suffers from severe recombination of electron–hole pairs at the interface, which greatly limits its application in photoelectrochemistry. To tackle this issue, heterostructured photoelectrodes with efficient cocatalysts should be rationally designed and fabricated, which are usually made by expensive and complicated atomic layer deposition methods (ALD). Herein, a facile chemical bath deposition (CBD) method is proposed to construct heterostructured photocathodes composed of TiO2 and Sb2Se3, as well as to deposit a cocatalyst of Pt nanoparticles (NPs) on the photoelectrode. The TiO2 layer could protect Sb2Se3 and also capture the photogenerated electrons produced by Sb2Se3, and then improve charge separation. Pt is utilized as a co-catalyst to enhance the carrier injection efficiency and hence accelerate the surface hydrogen evolution reaction. Under simulated sunlight conditions, Sb2Se3-5/TiO2-3/Pt-6 with the optimized configuration exhibited a flat band potential of 0.52 VRHE, which is positively shifted by 0.09 V with respect to that of bare Sb2Se3. Notably, photocurrent densities of −1.0 mA cm−2 at −0.2 VRHE and 0.56 mA cm−2 at 0 VRHE were achieved. This represented 12.5 and 7 times improvement in photocurrent densities compared to bare Sb2Se3 NPs. Our study provides a facile and effective method for the interface engineering of Sb2Se3, resulting in a significant enhancement of its photoelectrochemical activity for serving as a high-performance photocathode for solar water splitting.
{"title":"Interfacial engineering enabling solution-processed Cu:NiOx/Sb2Se3/TiO2/Pt photocathodes for highly efficient photoelectrochemical water-splitting†","authors":"Yinbo Zhan, Ying-Chu Chen and Xia Long","doi":"10.1039/D4SE00602J","DOIUrl":"10.1039/D4SE00602J","url":null,"abstract":"<p >Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small> is a promising photocathode with good stability and large theoretical photocurrent density but suffers from severe recombination of electron–hole pairs at the interface, which greatly limits its application in photoelectrochemistry. To tackle this issue, heterostructured photoelectrodes with efficient cocatalysts should be rationally designed and fabricated, which are usually made by expensive and complicated atomic layer deposition methods (ALD). Herein, a facile chemical bath deposition (CBD) method is proposed to construct heterostructured photocathodes composed of TiO<small><sub>2</sub></small> and Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small>, as well as to deposit a cocatalyst of Pt nanoparticles (NPs) on the photoelectrode. The TiO<small><sub>2</sub></small> layer could protect Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small> and also capture the photogenerated electrons produced by Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small>, and then improve charge separation. Pt is utilized as a co-catalyst to enhance the carrier injection efficiency and hence accelerate the surface hydrogen evolution reaction. Under simulated sunlight conditions, Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small>-5/TiO<small><sub>2</sub></small>-3/Pt-6 with the optimized configuration exhibited a flat band potential of 0.52 V<small><sub>RHE</sub></small>, which is positively shifted by 0.09 V with respect to that of bare Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small>. Notably, photocurrent densities of −1.0 mA cm<small><sup>−2</sup></small> at −0.2 V<small><sub>RHE</sub></small> and 0.56 mA cm<small><sup>−2</sup></small> at 0 V<small><sub>RHE</sub></small> were achieved. This represented 12.5 and 7 times improvement in photocurrent densities compared to bare Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small> NPs. Our study provides a facile and effective method for the interface engineering of Sb<small><sub>2</sub></small>Se<small><sub>3</sub></small>, resulting in a significant enhancement of its photoelectrochemical activity for serving as a high-performance photocathode for solar water splitting.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528026","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}
Fuqiang Zhang, Zhiqiang Qi, Xiangsheng Han, Hongzhen Cai and Keyan Yang
Interfacial solar steam generation (ISSG) is an effective method to produce clean water through evaporating seawater actuated by solar energy. Nevertheless, developing a solar evaporator that is simultaneously simple in process and maintains good stability and high efficiency is still difficult but in great demand. Herein, an aerogel solar evaporator was prepared by cross-linking chitosan (CS) and two-dimensional transition metal carbide/nitride (MXene) nanosheets with excellent properties via a simple freeze-drying strategy. The unique three-dimensional network structure and good biocompatibility could facilitate quick transport of water from the bottom up to the evaporation surface by capillary force. MXene nanosheets combined a broad spectral response with strong solar absorption capacity, enabling the CS/MXene aerogel solar evaporator to exhibit strong light absorption, light-to-heat conversion, and water transport capabilities. The results showed that the water evaporation rate under one sun was as high as 1.80 kg m−2 h−1, with an energy conversion efficiency of 75.2%. Notably, the stability of the solar evaporator ensured stable solar water evaporation over a long period compared with most CS-based solar evaporators. Meanwhile, clean water could be continuously produced from acidic, alkaline and organic dye solutions, and saline brines. These tactics pave a new way for developing solar absorbers for solar-driven desalination.
{"title":"MXene nanosheet-reinforced chitosan as a stable photothermal evaporator for efficient solar evaporation†","authors":"Fuqiang Zhang, Zhiqiang Qi, Xiangsheng Han, Hongzhen Cai and Keyan Yang","doi":"10.1039/D4SE00617H","DOIUrl":"10.1039/D4SE00617H","url":null,"abstract":"<p >Interfacial solar steam generation (ISSG) is an effective method to produce clean water through evaporating seawater actuated by solar energy. Nevertheless, developing a solar evaporator that is simultaneously simple in process and maintains good stability and high efficiency is still difficult but in great demand. Herein, an aerogel solar evaporator was prepared by cross-linking chitosan (CS) and two-dimensional transition metal carbide/nitride (MXene) nanosheets with excellent properties <em>via</em> a simple freeze-drying strategy. The unique three-dimensional network structure and good biocompatibility could facilitate quick transport of water from the bottom up to the evaporation surface by capillary force. MXene nanosheets combined a broad spectral response with strong solar absorption capacity, enabling the CS/MXene aerogel solar evaporator to exhibit strong light absorption, light-to-heat conversion, and water transport capabilities. The results showed that the water evaporation rate under one sun was as high as 1.80 kg m<small><sup>−2</sup></small> h<small><sup>−1</sup></small>, with an energy conversion efficiency of 75.2%. Notably, the stability of the solar evaporator ensured stable solar water evaporation over a long period compared with most CS-based solar evaporators. Meanwhile, clean water could be continuously produced from acidic, alkaline and organic dye solutions, and saline brines. These tactics pave a new way for developing solar absorbers for solar-driven desalination.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141529446","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}
Rational design of materials in a catalytic system is the main determinant of the efficiency of sustainable energy sources. Significant efforts have focused on the study and development of flatland two-dimensional (2D) materials (MXenes, MBenes, transition metal dichalcogenides/phosphides (TMDs/TMPs), phosphorene, graphene derivatives) towards energy-driven aspirations in consideration of their superior physiochemical properties as compared to their non-layered counterpart materials, surpassing their transport properties and conductivity. Herein, we aim to provide a detailed account of where the flatland materials currently stand to achieve the goal of sustainability in light of their photochemical and electrochemical nitrogen fixation applications. As of now, numerous challenges have limited the expansion of 2D-material derived nitrogen fixation operations for scalable applications. Therefore, we summarized techno-economic analysis and future perspectives of nitrogen fixation applications in relation to their practical ammonia applicability. We have briefly summarized the functionality of flatland materials and classified them on the basis of their photochemical and electrochemical efficiencies.
{"title":"Flatland materials for photochemical and electrochemical nitrogen fixation applications: from lab-door experiments to large-scale applicability","authors":"Syed Asim Ali, Iqra Sadiq and Tokeer Ahmad","doi":"10.1039/D4SE00565A","DOIUrl":"10.1039/D4SE00565A","url":null,"abstract":"<p >Rational design of materials in a catalytic system is the main determinant of the efficiency of sustainable energy sources. Significant efforts have focused on the study and development of flatland two-dimensional (2D) materials (MXenes, MBenes, transition metal dichalcogenides/phosphides (TMDs/TMPs), phosphorene, graphene derivatives) towards energy-driven aspirations in consideration of their superior physiochemical properties as compared to their non-layered counterpart materials, surpassing their transport properties and conductivity. Herein, we aim to provide a detailed account of where the flatland materials currently stand to achieve the goal of sustainability in light of their photochemical and electrochemical nitrogen fixation applications. As of now, numerous challenges have limited the expansion of 2D-material derived nitrogen fixation operations for scalable applications. Therefore, we summarized techno-economic analysis and future perspectives of nitrogen fixation applications in relation to their practical ammonia applicability. We have briefly summarized the functionality of flatland materials and classified them on the basis of their photochemical and electrochemical efficiencies.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528024","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}
Haozhe Zhang, Yanjie Wang, Wentian Niu, Tatchamapan Yoskamtorn, Mingyu Luo, Robert Tayler, Sarah Day and Shik Chi Edman Tsang
The augmentation of photocatalytic activity in layered perovskite oxides via the integration of graphene-like materials presents a promising pathway for the optimization of solar energy conversion. The electron-rich nature of graphene, coupled with its high electron conductivity, functions as an effective photosensitizer, thereby enhancing visible light harvesting. In this investigation, we have, for the first time, assembled ultrathin exfoliated Dion–Jacobson perovskite layers with reduced graphene oxide (rGO) layers, resulting in a high surface area layered nanocomposite, achieved through a tailored electrostatic approach. To further refine the electron properties of the layered perovskite–reduced graphene oxide composites, we have explored the use of various lanthanides as A-site cations in the Dion–Jacobson perovskites, including LaNb2O7 (LNO), PrNb2O7 (PNO), and NdNb2O7 (NNO). The synthesized composites demonstrate exceptional performance in photocatalytic H2 production, with rGO/NNO exhibiting the highest activity, achieving a hydrogen evolution rate (HER) of 835 μmol g−1 under light illumination, attributable to optimal interfacial effects. Our experimental and theoretical analyses indicate that hydrogen production is predominantly influenced by the A-site cation charge density at the materials' interface, as dictated by the charge transfer dynamics. This research potentially contributes to the comprehension and enhancement of photocatalytic processes for applications in solar energy conversion.
通过整合类石墨烯材料来增强层状过氧化物的光催化活性,为优化太阳能转换提供了一条前景广阔的途径。石墨烯富含电子的特性与其高电子传导性相结合,可作为一种有效的光敏剂,从而提高可见光的收集能力。在这项研究中,我们首次将超薄剥离的 Dion-Jacobson 包晶石层与还原氧化石墨烯(rGO)层组装在一起,通过定制的静电方法获得了高比表面积的层状纳米复合材料。为了进一步完善层状包晶石-还原氧化石墨烯复合材料的电子特性,我们探索了在狄昂-矢量包晶石中使用各种镧系元素作为 A 位阳离子,包括 LaNb2O7 (LNO)、PrNb2O7 (PNO) 和 NdNb2O7 (NNO)。合成的复合材料在光催化产氢方面表现出卓越的性能,其中 rGO/NNO 的活性最高,在光照下的氢进化率(HER)达到 835 μmol g-1,这归功于最佳的界面效应。我们的实验和理论分析表明,制氢主要受材料界面上 A 位阳离子电荷密度的影响,这是由电荷转移动力学决定的。这项研究可能有助于理解和加强光催化过程在太阳能转换中的应用。
{"title":"Tuning 2D perovskite–graphene layered composite for photocatalysis†","authors":"Haozhe Zhang, Yanjie Wang, Wentian Niu, Tatchamapan Yoskamtorn, Mingyu Luo, Robert Tayler, Sarah Day and Shik Chi Edman Tsang","doi":"10.1039/D4SE00630E","DOIUrl":"10.1039/D4SE00630E","url":null,"abstract":"<p >The augmentation of photocatalytic activity in layered perovskite oxides <em>via</em> the integration of graphene-like materials presents a promising pathway for the optimization of solar energy conversion. The electron-rich nature of graphene, coupled with its high electron conductivity, functions as an effective photosensitizer, thereby enhancing visible light harvesting. In this investigation, we have, for the first time, assembled ultrathin exfoliated Dion–Jacobson perovskite layers with reduced graphene oxide (rGO) layers, resulting in a high surface area layered nanocomposite, achieved through a tailored electrostatic approach. To further refine the electron properties of the layered perovskite–reduced graphene oxide composites, we have explored the use of various lanthanides as A-site cations in the Dion–Jacobson perovskites, including LaNb<small><sub>2</sub></small>O<small><sub>7</sub></small> (LNO), PrNb<small><sub>2</sub></small>O<small><sub>7</sub></small> (PNO), and NdNb<small><sub>2</sub></small>O<small><sub>7</sub></small> (NNO). The synthesized composites demonstrate exceptional performance in photocatalytic H<small><sub>2</sub></small> production, with rGO/NNO exhibiting the highest activity, achieving a hydrogen evolution rate (HER) of 835 μmol g<small><sup>−1</sup></small> under light illumination, attributable to optimal interfacial effects. Our experimental and theoretical analyses indicate that hydrogen production is predominantly influenced by the A-site cation charge density at the materials' interface, as dictated by the charge transfer dynamics. This research potentially contributes to the comprehension and enhancement of photocatalytic processes for applications in solar energy conversion.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/se/d4se00630e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528022","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}
Palanivel Subha, Kumar Krishan and Putla Sudarsanam
Valorization of lignocellulosic biomass, an abundantly available renewable hydrocarbon source, to produce value-added chemicals, drop-in chemicals, and biofuels is indispensable, considering the limited sources of fossil fuels and their adverse environmental effects. The application of efficient heterogeneous catalysts is a promising method of sustainable biomass processing with low energy consumption and minimal waste generation. Hydroprocessing of biomass using a hydrogen source is considered to be a pivotal strategy for the synthesis of industrially important chemicals and fuels. As the use of molecular hydrogen gas results in several problems and requires harsh reaction conditions, the utilization of safe and clean liquid hydrogen carriers is preferred to address the economic and sustainable aspects of biorefinery. In this review, we address the significance of in situ hydrogen generation for biomass hydroprocessing. The primary focus of the review is the catalytic transfer hydrogenation (CTH) of lignocellulosic biomass-derived molecules using various liquid hydrogen carriers. Various heterogeneous catalysts, including bulk, nanosized, and single-atom catalysts, and the role of their BET surface area, pore size, particle size/morphology, surface chemistry, acid–base, and redox properties in biomass hydrogenation to obtain desirable products are meticulously discussed with the support of kinetic, mechanistic, and theoretical studies. The challenges associated with the in situ generation of hydrogen and its selective adsorption/activation on the catalyst surface for the CTH processing of biomass-derived molecules as well as the prospects for a rational design of novel heterogeneous catalysts and the utilization of new hydrogen carriers for biomass valorization are elucidated.
木质纤维素生物质是一种丰富的可再生碳氢化合物来源,考虑到化石燃料来源有限及其对环境的不利影响,对其进行增值处理以生产增值化学品、无须添加的化学品和生物燃料是必不可少的。应用高效的异相催化剂是实现可持续生物质加工、低能耗和最少废物产生的一种可行方法。利用氢源对生物质进行水处理被认为是合成工业重要化学品和燃料的关键策略。由于分子氢气的使用会带来一些不明确的问题,并且需要苛刻的反应条件,因此利用安全、清洁的液氢前体是解决生物炼制的经济性和可持续性问题的首选。在本综述中,我们探讨了原位制氢对生物质加氢处理的重要意义。综述的主要重点是使用各种液氢载体对木质纤维素生物质衍生分子进行催化转移加氢 (CTH)。在动力学、机理和理论研究的支持下,详细讨论了各种异质催化剂(包括块状、纳米和单原子催化剂)及其 BET 表面积、孔径、粒径/形态、表面化学、酸碱和氧化还原特性在生物质加氢以获得理想产物中的作用。此外,还阐明了与原位生成氢及其在催化剂表面的选择性吸附/活化有关的挑战,以及合理设计新型异相催化剂和利用新型氢载体实现生物质增值的前景。
{"title":"In situ hydroprocessing of lignocellulosic biomass-derived molecules into fuels and chemicals using heterogeneous catalysts","authors":"Palanivel Subha, Kumar Krishan and Putla Sudarsanam","doi":"10.1039/D4SE00666F","DOIUrl":"10.1039/D4SE00666F","url":null,"abstract":"<p >Valorization of lignocellulosic biomass, an abundantly available renewable hydrocarbon source, to produce value-added chemicals, drop-in chemicals, and biofuels is indispensable, considering the limited sources of fossil fuels and their adverse environmental effects. The application of efficient heterogeneous catalysts is a promising method of sustainable biomass processing with low energy consumption and minimal waste generation. Hydroprocessing of biomass using a hydrogen source is considered to be a pivotal strategy for the synthesis of industrially important chemicals and fuels. As the use of molecular hydrogen gas results in several problems and requires harsh reaction conditions, the utilization of safe and clean liquid hydrogen carriers is preferred to address the economic and sustainable aspects of biorefinery. In this review, we address the significance of <em>in situ</em> hydrogen generation for biomass hydroprocessing. The primary focus of the review is the catalytic transfer hydrogenation (CTH) of lignocellulosic biomass-derived molecules using various liquid hydrogen carriers. Various heterogeneous catalysts, including bulk, nanosized, and single-atom catalysts, and the role of their BET surface area, pore size, particle size/morphology, surface chemistry, acid–base, and redox properties in biomass hydrogenation to obtain desirable products are meticulously discussed with the support of kinetic, mechanistic, and theoretical studies. The challenges associated with the <em>in situ</em> generation of hydrogen and its selective adsorption/activation on the catalyst surface for the CTH processing of biomass-derived molecules as well as the prospects for a rational design of novel heterogeneous catalysts and the utilization of new hydrogen carriers for biomass valorization are elucidated.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141528028","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}
Jun Shu, Jianqin Fu, Wenhui Yang, Jianxiang Huang, Tingpu He and Jingping Liu
This study investigates the impact of diesel pilot ignition (DPI) natural gas (NG) engines on combustion and emission characteristics across various exhaust gas recirculation (EGR) volumes. It utilizes a three-dimensional computational fluid dynamics (CFD) model coupled with a simplified chemical kinetic model. Experimental results guide simulation calculations under three distinct operational conditions. Visual analysis of the calculation outcomes presents the combustion process and emission characteristics in the engine, elucidating the influence mechanism in relation to EGR volume rates. The simulation results show that, with the rise of EGR rates, the peak in-cylinder pressure decreases by 15 bar, the heat release rate (HRR) shoots up later, and the maximum difference of CA50 is less than 2.7 °CA. The variation trends of CA90, 50–90% and 10–90% combustion durations exhibit similarity. When the rate of EGR volume is below 20%, the CA90, 50–90%, and 10–90% combustion durations lengthen as the rate of EGR volume increases. When the rate of EGR volume exceeds 20%, NOx emissions remain at a low level, staying below 500 ppm. Concurrently, as the rate of EGR volume increases from 5% to 30%, there is a corresponding rise in unburned methane emissions, with the maximum surge observed from 343 ppm to 21 021 ppm. Additionally, CO emissions increase as the rate of EGR volume increases, reaching 989 ppm in case 3. While in case 2, there is an initial ascent to 1381 ppm, followed by a decline to 1148 ppm, and ultimately, a subsequent rise.
{"title":"Experimental and computational study on the effects of exhaust gas recirculation on thermodynamics, combustion and emission characteristics of a diesel pilot ignition natural gas engine","authors":"Jun Shu, Jianqin Fu, Wenhui Yang, Jianxiang Huang, Tingpu He and Jingping Liu","doi":"10.1039/D4SE00635F","DOIUrl":"10.1039/D4SE00635F","url":null,"abstract":"<p >This study investigates the impact of diesel pilot ignition (DPI) natural gas (NG) engines on combustion and emission characteristics across various exhaust gas recirculation (EGR) volumes. It utilizes a three-dimensional computational fluid dynamics (CFD) model coupled with a simplified chemical kinetic model. Experimental results guide simulation calculations under three distinct operational conditions. Visual analysis of the calculation outcomes presents the combustion process and emission characteristics in the engine, elucidating the influence mechanism in relation to EGR volume rates. The simulation results show that, with the rise of EGR rates, the peak in-cylinder pressure decreases by 15 bar, the heat release rate (HRR) shoots up later, and the maximum difference of CA50 is less than 2.7 °CA. The variation trends of CA90, 50–90% and 10–90% combustion durations exhibit similarity. When the rate of EGR volume is below 20%, the CA90, 50–90%, and 10–90% combustion durations lengthen as the rate of EGR volume increases. When the rate of EGR volume exceeds 20%, NOx emissions remain at a low level, staying below 500 ppm. Concurrently, as the rate of EGR volume increases from 5% to 30%, there is a corresponding rise in unburned methane emissions, with the maximum surge observed from 343 ppm to 21 021 ppm. Additionally, CO emissions increase as the rate of EGR volume increases, reaching 989 ppm in case 3. While in case 2, there is an initial ascent to 1381 ppm, followed by a decline to 1148 ppm, and ultimately, a subsequent rise.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141506690","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}