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Performances and Mechanisms of Dehydration of Levoglucosan to Levoglucosenone over Cesium Heterpolyacid Salts 左旋葡聚糖在铯杂多酸盐上脱水成左旋葡塞酮的性能和机理
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-09 DOI: 10.1021/acs.energyfuels.4c0412810.1021/acs.energyfuels.4c04128
Xin Huang*, Guangchuan Tang, Lei Tang, Chuan Ma, Yunlin Shao and Jingyu Ran, 

Bio-based platform chemicals are of great significance to future green fine and commodity chemicals. This study reports the performances and mechanisms of solvothermal dehydration of levoglucosan (LGA), the main precursor from noncatalytic pyrolysis of cellulose with a yield up to 80 wt %, to levoglucosenone (LGO) using cesium heteropolyacid salts at the catalyst in DMSO solvent. Catalyst characterizations revealed that cesium was well doped in the cubic of heteropolyacids, and the cesium doping ratio substantially influenced the catalytic performances toward LGO. LGO yield first increased and then decreased with the increase of cesium doping ratios, which is consistent with the change trends of pore structures and Brønsted/Lewis acid site ratios of the cesium heteropolyacid salts. LGO was obtained with the maximum yield at 41.2% over Cs2H2SiW12O40 compared to 39.2% over Cs2.5H0.5PW12O40. The catalyst can be regenerated by calcination without losing its catalytic performances. In addition, density functional theory calculation was used to reveal the mechanism for LGO formation, and the rate-determining step was the first step of the dehydration reaction with the energy barrier of 166 kJ/mol.

生物基平台化学品对未来的绿色精细化学品和商品化学品具有重要意义。本研究报告了在 DMSO 溶剂中,以铯杂多酸盐为催化剂,对纤维素非催化热解产生的主要前体物左旋葡聚糖(LGA)进行溶热脱水生成左旋葡塞酮(LGO)的性能和机理。催化剂表征显示,铯在杂多酸的立方体中掺杂良好,铯的掺杂率极大地影响了催化剂对 LGO 的催化性能。随着铯掺杂比的增加,LGO产率先升后降,这与铯杂多酸盐的孔结构和布氏/路易斯酸位点比的变化趋势一致。与 Cs2.5H0.5PW12O40 的 39.2%相比,Cs2H2SiW12O40 得到的 LGO 产率最高,达到 41.2%。该催化剂可通过煅烧再生,而不会丧失其催化性能。此外,还利用密度泛函理论计算揭示了 LGO 的形成机理,其中决定速率的步骤是脱水反应的第一步,能垒为 166 kJ/mol。
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引用次数: 0
A Critical Review on the Structure and Recovery Technologies of End-of-Life Wind Turbine Blades 关于报废风力涡轮机叶片结构和回收技术的重要评论
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0364810.1021/acs.energyfuels.4c03648
Zefeng Ge, Yuqing Wu, Mingxun Zeng and Huiyan Zhang*, 

Wind power technology, as a crucial form of wind energy application, is one of the most mature generation methods in the global renewable energy sector. With the rapid growth of wind power, early generation wind turbines are approaching their decommissioning peak, resulting in a large volume of end-of-life wind turbine blades (EWTBs). The recycling and resource utilization of EWTBs represent a new and significant research area that could help achieve a sustainable future while reducing waste. This work focuses on efficient recycling and resource utilization of EWTBs, particularly concerning organic resins and inorganic fibers. Traditional disposal methods, such as landfilling and incineration, result in severe resource waste and environmental pollution. Therefore, the development of clean and efficient recycling solutions is imperative. To provide a comprehensive understanding of current recycling practices, this paper reviews the composition, properties, and utilization technologies of EWTBs. It systematically introduces various recycling techniques, including physical, electric-driven, thermal, and chemical recycling methods. The progress of different technologies is analyzed, with thermal conversion recycling emerging as the most promising due to its rapid conversion rate and wide feedstock applicability. Furthermore, the paper evaluates the applications of thermal-chemical recycling products. It emphasizes that future recycling methods should focus on low-temperature processing and multienergy coupling concepts. The policy adjustments will significantly impact the applicability and economic feasibility of EWTBs recycling technologies. Sustainable utilization of EWTBs necessitates collaboration among government agencies, manufacturers, and technical departments, representing a trend toward large-scale recycling of EWTBs and ensuring the efficient, environmental, and green circular development of the wind power generation industry.

风力发电技术作为风能应用的重要形式,是全球可再生能源领域最成熟的发电方式之一。随着风力发电的快速发展,早期风力涡轮机已接近退役高峰,从而产生了大量报废风力涡轮机叶片(EWTB)。EWTBs 的回收和资源利用是一个新的重要研究领域,有助于在减少浪费的同时实现可持续发展的未来。这项工作的重点是 EWTB 的高效回收和资源利用,尤其是有机树脂和无机纤维。填埋和焚烧等传统处理方法会造成严重的资源浪费和环境污染。因此,开发清洁高效的回收解决方案势在必行。为了全面了解当前的回收实践,本文回顾了 EWTB 的成分、特性和利用技术。它系统地介绍了各种回收技术,包括物理、电驱动、热和化学回收方法。分析了不同技术的进展,其中热转换回收技术因其转换速度快、原料适用性广而成为最有前景的技术。此外,论文还对热化学回收产品的应用进行了评估。论文强调,未来的回收方法应侧重于低温处理和多能源耦合概念。政策调整将极大地影响 EWTBs 循环利用技术的适用性和经济可行性。EWTBs 的可持续利用需要政府机构、制造商和技术部门的通力合作,这也是 EWTBs 大规模回收利用的趋势,确保风力发电行业高效、环保、绿色的循环发展。
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引用次数: 0
Fast and ex Situ Catalytic Copyrolysis of Switchgrass and Waste Polyethylene 快速原位催化复制分解开关草和废聚乙烯
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0351010.1021/acs.energyfuels.4c03510
Charles A. Mullen*, Gary D. Strahan, Yaseen Elkasabi and Candice Ellison, 

Continuous fast and ex situ catalytic pyrolysis of blends of switchgrass with 15 wt % polyethylene (PE) was studied using a fluidized bed pyrolysis system. Higher than typical temperatures for biomass pyrolysis were utilized (630 °C) to overcome the higher thermal stability of polyethylene. For fast pyrolysis, the high pyrolysis temperature led to a lower yield of oil and a higher yield of gas from the switchgrass. When polyethylene was blended in, a small increase in the yield of oil was noted, and the oil had a slightly lower oxygen content and higher hydrogen content. GC/MS and NMR analysis showed that linear alkenes and alkanes were present in the oil in addition to phenolics, acids, and other oxygenates derived from biomass. However, a phase separated wax product was also formed, and this accounted for an estimated 27% of the input plastic carbon. Ethylene was also a major product of PE pyrolysis, accounting for 29% of the input plastic carbon. Only about 19% of the input plastic carbon was in the oil product. When ex situ catalytic pyrolysis was performed over HY at 250 °C, the oil product phase separated into a largely biomass derived fraction and a plastic derived fraction. When the catalysis was performed at 300 °C, there was a shift in reactivity for the blends compared with switchgrass only, decreasing CO formation and resulting in an oil rich in alkyl benzenes, alkyl naphthalenes, and alkyl phenols.

利用流化床热解系统研究了开关草与 15 wt % 聚乙烯(PE)混合物的连续快速原位催化热解。为了克服聚乙烯较高的热稳定性,生物质热解采用了比一般温度更高的温度(630 °C)。在快速热解过程中,高热解温度导致开关草的产油量降低,产气量增加。掺入聚乙烯后,油的产量略有增加,油中的氧含量略低,氢含量较高。气相色谱/质谱和核磁共振分析表明,除了酚类、酸类和其他从生物质中提取的含氧化合物外,油中还含有直链烯和烷烃。不过,还形成了一种相分离的蜡产品,估计占输入塑料碳的 27%。乙烯也是聚乙烯热解的主要产物,占输入塑料碳的 29%。只有约 19% 的输入塑料碳存在于油产品中。在 250 °C 的温度下对 HY 进行原位催化热解时,油产品相分离成主要由生物质衍生的部分和由塑料衍生的部分。当催化温度为 300 °C时,与仅使用开关草相比,混合物的反应性发生了变化,减少了一氧化碳的形成,并产生了富含烷基苯、烷基萘和烷基酚的油。
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引用次数: 0
2024 Energy and Fuels Rising Stars 2024 能源与燃料新星
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0459510.1021/acs.energyfuels.4c04595
Hongwei Wu, 
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引用次数: 0
Kinetic Modeling of Hydrogen Generation via In Situ Combustion Gasification of Heavy Oil 重油原位燃烧气化制氢的动力学建模
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0323710.1021/acs.energyfuels.4c03237
Mohamed Amine Ifticene, Yunan Li, Ping Song and Qingwang Yuan*, 

In the global push for sustainable energy, in situ combustion gasification (ISCG) has emerged as a transformative technology to leverage the world’s abundant heavy oil reserves for producing carbon-zero hydrogen. Chemical kinetics are crucial for modeling subsurface hydrogen generation and optimizing production schemes to maximize hydrogen yield, which are however currently lacking. This study aims to develop the first experimentally validated kinetic model for hydrogen generation during ISCG of heavy oil. To accurately model ISCG reactions, particularly hydrogen generation, we combined kinetic cell experiments with numerical modeling to history match the experimental results. The temporal variation of generated gases, such as hydrogen, measured in laboratory experiments, served as the baseline for history matching. A differential evolution optimization algorithm was employed to calibrate the kinetic parameters of the numerical model with experimental results. The kinetic model for combustion reactions was accurately calibrated after 454 optimization runs with a history-matching error of 3.46%. This accuracy is attributed to the well-studied nature of heavy oil oxidation and the comprehensive reaction scheme employed. Conversely, calibrating the kinetic model for gasification reactions with kinetic cell experimental results proved more challenging yielding a history-matching error of 22.19% after 488 optimization runs. Despite significant uncertainties in hydrogen generation and consumption reactions due to limited knowledge of the gasification process, our proposed kinetic model can still predict hydrogen generation with a simplified but powerful reaction scheme, compared to previously proposed ISCG models that involve numerous reactions. This work introduces the first kinetic model to describe the hydrogen generation process during ISCG of heavy oil with rigorous experimental validation. This reliable kinetic model establishes a solid foundation for future multiscale reservoir simulation and further optimization of the field development for enhanced hydrogen production in a more sustainable manner.

在全球推动可持续能源发展的过程中,原地燃烧气化(ISCG)已成为一项变革性技术,可利用全球丰富的重油储量生产零碳氢气。化学动力学对于建立地下氢气生成模型和优化生产方案以最大限度地提高氢气产量至关重要,但目前还缺乏这方面的研究。本研究旨在为重油 ISCG 过程中的氢气生成建立首个经过实验验证的动力学模型。为了准确模拟 ISCG 反应,特别是氢气生成,我们将动力学电池实验与数值建模相结合,使其与实验结果相吻合。实验室实验中测得的氢气等生成气体的时间变化是历史匹配的基准。采用差分进化优化算法将数值模型的动力学参数与实验结果进行校准。经过 454 次优化运行后,燃烧反应动力学模型得到了精确校准,历史匹配误差为 3.46%。这一准确性归功于对重油氧化的深入研究和所采用的全面反应方案。相反,用动力学电池实验结果校准气化反应动力学模型则更具挑战性,经过 488 次优化运行后,历史匹配误差达到 22.19%。尽管由于对气化过程的了解有限,氢气生成和消耗反应存在很大的不确定性,但与之前提出的涉及众多反应的 ISCG 模型相比,我们提出的动力学模型仍能通过简化但功能强大的反应方案预测氢气生成。这项研究首次提出了描述重油 ISCG 制氢过程的动力学模型,并经过了严格的实验验证。这一可靠的动力学模型为未来的多尺度油藏模拟和进一步优化油田开发奠定了坚实的基础,从而以更可持续的方式提高氢气产量。
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引用次数: 0
Pore-Fissure Compressibility and Structural Dynamic Evolution of Coal Reservoir under Confining Pressure 封闭压力下煤储层孔隙压缩性与结构动态演化
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0307210.1021/acs.energyfuels.4c03072
Dameng Liu*, Bo Zhao, Jin Cui, Yidong Cai, Fengrui Sun, Bingyi Wang and Yingfang Zhou, 

Coal reservoirs exhibit a ternary structure comprising pores, microfissures, and macro-fissures, crucial for determining permeability and influencing the adsorption–desorption–diffusion–seepage processes of coalbed methane (CBM). These factors significantly impact the CBM recoverability and production. Through dynamic permeability experiments, nuclear magnetic resonance (NMR) under varied confining pressures, and triaxial compression-CT scanning, the stress sensitivity of coal in different directions under varying confining pressures, pore pressures, and effective stress conditions was investigated. It is obtained that (1) the stress sensitivity of coal fissures is notably high, and they tend to close first under confining pressure. Seepage and adsorption pores exhibit two trends: a gradual decrease or an initial increase followed by a decrease. With deeper coal metamorphism, the stress sensitivity of fissures gradually diminishes, while the stress sensitivity of adsorption pores increases. (2) The fissure compressibility measured by He is the lowest, CO2 is always the highest, and CH4 is between the two. The fissure compressibility measured by He decreases exponentially with the increase of pore pressure, while the adsorbed gases CH4 and CO2 change complicatedly, decreasing exponentially, or parabolically. (3) The significant stress sensitivity and permeability damage rate occur in the direction of parallel-face cuttings of experimental coals, while the vertical direction exhibits the weakest characteristics. Nonhomogeneity is most pronounced between these two directions. The anisotropy of the coal reservoir diminishes gradually with increasing peripheral pressure.

煤储层呈现出由孔隙、微裂隙和大裂隙组成的三元结构,这对于决定渗透性和影响煤层气的吸附-解吸-扩散-渗流过程至关重要。这些因素对煤层气的可采性和产量有着重大影响。通过动态渗透实验、不同约束压力下的核磁共振(NMR)和三轴压缩 CT 扫描,研究了煤在不同约束压力、孔隙压力和有效应力条件下不同方向的应力敏感性。结果表明:(1) 煤裂隙的应力敏感性明显较高,在封闭压力作用下有先闭合的趋势。渗孔和吸附孔呈现两种趋势:逐渐减少或先增加后减少。随着煤变质程度的加深,裂隙的应力敏感性逐渐减弱,而吸附孔隙的应力敏感性则逐渐增强。(2)用 He 测量的裂隙压缩性最低,CO2 始终最高,CH4 介于两者之间。He 测得的裂隙可压缩性随孔隙压力的增加呈指数下降,而吸附气体 CH4 和 CO2 的变化复杂,有的呈指数下降,有的呈抛物线下降。(3)应力敏感性和渗透破坏率在实验煤的平行面切割方向上表现出明显的特征,而在垂直方向上表现出最弱的特征。这两个方向之间的非均质性最为明显。煤储层的各向异性随着周边压力的增加而逐渐减弱。
{"title":"Pore-Fissure Compressibility and Structural Dynamic Evolution of Coal Reservoir under Confining Pressure","authors":"Dameng Liu*,&nbsp;Bo Zhao,&nbsp;Jin Cui,&nbsp;Yidong Cai,&nbsp;Fengrui Sun,&nbsp;Bingyi Wang and Yingfang Zhou,&nbsp;","doi":"10.1021/acs.energyfuels.4c0307210.1021/acs.energyfuels.4c03072","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c03072https://doi.org/10.1021/acs.energyfuels.4c03072","url":null,"abstract":"<p >Coal reservoirs exhibit a ternary structure comprising pores, microfissures, and macro-fissures, crucial for determining permeability and influencing the adsorption–desorption–diffusion–seepage processes of coalbed methane (CBM). These factors significantly impact the CBM recoverability and production. Through dynamic permeability experiments, nuclear magnetic resonance (NMR) under varied confining pressures, and triaxial compression-CT scanning, the stress sensitivity of coal in different directions under varying confining pressures, pore pressures, and effective stress conditions was investigated. It is obtained that (1) the stress sensitivity of coal fissures is notably high, and they tend to close first under confining pressure. Seepage and adsorption pores exhibit two trends: a gradual decrease or an initial increase followed by a decrease. With deeper coal metamorphism, the stress sensitivity of fissures gradually diminishes, while the stress sensitivity of adsorption pores increases. (2) The fissure compressibility measured by He is the lowest, CO<sub>2</sub> is always the highest, and CH<sub>4</sub> is between the two. The fissure compressibility measured by He decreases exponentially with the increase of pore pressure, while the adsorbed gases CH<sub>4</sub> and CO<sub>2</sub> change complicatedly, decreasing exponentially, or parabolically. (3) The significant stress sensitivity and permeability damage rate occur in the direction of parallel-face cuttings of experimental coals, while the vertical direction exhibits the weakest characteristics. Nonhomogeneity is most pronounced between these two directions. The anisotropy of the coal reservoir diminishes gradually with increasing peripheral pressure.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450862","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Self-Energized Pyrolysis Process for Sustainable Biochar Production 用于可持续生物炭生产的自发电热解工艺
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-08 DOI: 10.1021/acs.energyfuels.4c0303910.1021/acs.energyfuels.4c03039
Javier Ordonez-Loza, Hanieh Bamdad, Sara Spataro, Sadegh Papari and Franco Berruti*, 

Biochar has sparked interest as a strategy for carbon capture and sequestration to offset carbon dioxide emissions, along with its various applications such as soil amendment, filler, catalyst, food/feed additive, or adsorbent. This interest is not merely a media-driven opportunity, but also stems from the ample availability of residual biomass and organic waste that can be transformed and integrated into production chains to reduce their environmental footprint. However, this interest attracts the adoption of production technologies that, while meeting the goal of carrying out the pyrolysis process, need to be environmentally sustainable. In this paper, a model based on laboratory-scale experimentation results is proposed and three fundamental stages of the industrial pyrolysis process for the sole production of biochar are explored: drying, pyrolysis itself, and the combustion of gases and vapors as an energy source. In this scenario, the production of pyrolysis liquids is avoided, eliminating the need for condensation equipment, reducing operating costs, and preventing handling problems and potential contamination of the biochar. Three types of biomasses were used experimentally to evaluate the yields and characteristics of the pyrolysis products: cocoa bean shells, white spruce bark, and poplar bark. Cocoa bean shells were then selected to investigate the sensitivity of the main model parameters. The study demonstrates that the combustion of gases and vapors produced during the pyrolysis process of dried feedstocks generates sufficient energy to sustain the process itself. The efficiency of the combustion process, the heat transfer to the pyrolysis reactor, and the input moisture of the biomass feedstock represent the critical parameters affecting the thermal sustainability of the process.

生物炭作为一种碳捕集与封存战略,可抵消二氧化碳排放,同时还可用于土壤改良、填料、催化剂、食品/饲料添加剂或吸附剂等多种用途,因此引发了人们的兴趣。这种兴趣不仅仅是媒体推动的机遇,还源于大量的残余生物质和有机废物,它们可以转化并融入生产链,以减少对环境的影响。然而,这种兴趣吸引了生产技术的采用,这些技术在满足热解过程目标的同时,还需要具有环境可持续性。本文提出了一个基于实验室规模实验结果的模型,并探讨了仅生产生物炭的工业热解过程的三个基本阶段:干燥、热解本身以及作为能源的气体和蒸汽燃烧。在这一方案中,避免了热解液的生产,无需冷凝设备,降低了运营成本,并避免了处理问题和生物炭的潜在污染。实验中使用了三种生物质来评估热解产物的产量和特性:可可豆壳、白云杉树皮和杨树树皮。然后选择可可豆壳来研究主要模型参数的敏感性。研究表明,干燥原料在热解过程中产生的气体和蒸汽燃烧产生的能量足以维持热解过程本身。燃烧过程的效率、热解反应器的热传导以及生物质原料的输入水分是影响该过程热可持续性的关键参数。
{"title":"Self-Energized Pyrolysis Process for Sustainable Biochar Production","authors":"Javier Ordonez-Loza,&nbsp;Hanieh Bamdad,&nbsp;Sara Spataro,&nbsp;Sadegh Papari and Franco Berruti*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0303910.1021/acs.energyfuels.4c03039","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c03039https://doi.org/10.1021/acs.energyfuels.4c03039","url":null,"abstract":"<p >Biochar has sparked interest as a strategy for carbon capture and sequestration to offset carbon dioxide emissions, along with its various applications such as soil amendment, filler, catalyst, food/feed additive, or adsorbent. This interest is not merely a media-driven opportunity, but also stems from the ample availability of residual biomass and organic waste that can be transformed and integrated into production chains to reduce their environmental footprint. However, this interest attracts the adoption of production technologies that, while meeting the goal of carrying out the pyrolysis process, need to be environmentally sustainable. In this paper, a model based on laboratory-scale experimentation results is proposed and three fundamental stages of the industrial pyrolysis process for the sole production of biochar are explored: drying, pyrolysis itself, and the combustion of gases and vapors as an energy source. In this scenario, the production of pyrolysis liquids is avoided, eliminating the need for condensation equipment, reducing operating costs, and preventing handling problems and potential contamination of the biochar. Three types of biomasses were used experimentally to evaluate the yields and characteristics of the pyrolysis products: cocoa bean shells, white spruce bark, and poplar bark. Cocoa bean shells were then selected to investigate the sensitivity of the main model parameters. The study demonstrates that the combustion of gases and vapors produced during the pyrolysis process of dried feedstocks generates sufficient energy to sustain the process itself. The efficiency of the combustion process, the heat transfer to the pyrolysis reactor, and the input moisture of the biomass feedstock represent the critical parameters affecting the thermal sustainability of the process.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Simulation Study on the All-Inorganic CsSnxGe1–xI3-Based Perovskite Solar Cells Using Isotypic Perovskites as Hole Transport Layers 以同种包晶为空穴传输层的全无机 CsSnxGe1-xI3 基包晶太阳能电池模拟研究
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-07 DOI: 10.1021/acs.energyfuels.4c0396010.1021/acs.energyfuels.4c03960
Shuo Lin, Baoping Zhang, Weichao Wang, Tie-Yu Lü, Jinrong Zhou, Xiuyan Li, Yuhong Fang and Jin-Cheng Zheng*, 

All-inorganic Sn–Ge-based perovskite solar cells (PSCs) have made great progress in recent years. Furthermore, they can be used as promising lead-free absorbers for PSCs, and p-type-doped CsSnI3, CsGeI3, and CsSn0.5Ge0.5I3 could also be used as good hole transport layers (HTLs). In this simulation work, CsSnI3, CsGeI3, and CsSn0.5Ge0.5I3 are used as both absorbers and HTLs. The effects of the dopant concentration of HTLs, the thickness of absorbers, and HTLs on the photovoltaic performance of PSCs were studied to optimize the device structures. The maximum efficiencies from high to low are 28.35%, 26.35%, 25.84%, 25.23%, 18.83%, 17.49%, and 11.79% for the TiO2/i-CsSnI3/p-CsSnI3, TiO2/i-CsSn0.5Ge0.5I3/p-CsSn0.5Ge0.5I3, TiO2/i-CsSn0.5Ge0.5I3/p-CsSnI3, TiO2/i-CsSnI3/p-CsGeI3, TiO2/i-CsSn0.5Ge0.5I3/p-CsGeI3, TiO2/i-CsGeI3/p-CsGeI3, and TiO2/i-CsGeI3/p-CsSnI3, respectively. The TiO2/i-CsGeI3/p-CsSnI3 cell exhibits the lowest efficiency of 11.79% in all of the simulated PSCs due to the spike-like band offset at the i-CsGeI3/p-CsSnI3 interface and high recombination rate in the p-CsSnI3 region. It is found that the n-p structures could have better photovoltaic performance (thickness of i-film approaching zero) than the conventional n-i-p structures for the TiO2/i-CsSnI3/p-CsSnI3, TiO2/i-CsGeI3/p-CsGeI3, and TiO2/i-CsSn0.5Ge0.5I3/p-CsSn0.5Ge0.5I3 PSCs if the defects in HTLs created by high doping can be effectively controlled. The efficiencies of PSCs are sensitive to the defect density and defect level position, and the influence of defect density on the PV performance is larger than that of the defect level position. The solar cells could maintain high power conversion efficiency for defect density below about 5 × 1017 cm–3. Furthermore, the increase of the interface trap density is found to reduce the photovoltaic performance of PSCs. Our study provides insight into the optimal design of CsSnxGe1–xI3-based PSCs.

近年来,以锡-锗为基础的全无机包晶太阳能电池(PSCs)取得了长足的进步。此外,它们还可用作 PSCs 的无铅吸收体,而 p 型掺杂的 CsSnI3、CsGeI3 和 CsSn0.5Ge0.5I3 还可用作良好的空穴传输层(HTL)。在这项模拟工作中,CsSnI3、CsGeI3 和 CsSn0.5Ge0.5I3 被用作吸收体和 HTL。研究了 HTL 的掺杂浓度、吸收体和 HTL 的厚度对 PSCs 光伏性能的影响,以优化器件结构。5Ge0.5I3、TiO2/i-CsSn0.5Ge0.5I3/p-CsSnI3、TiO2/i-CsSnI3/p-CsGeI3、TiO2/i-CsSn0.5Ge0.5I3/p-CsGeI3、TiO2/i-CsGeI3/p-CsGeI3 和 TiO2/i-CsGeI3/p-CsSnI3。在所有模拟的 PSC 中,TiO2/i-CsGeI3/p-CsSnI3 电池的效率最低,仅为 11.79%,这是由于 i-CsGeI3/p-CsSnI3 界面的尖峰状带偏移和 p-CsSnI3 区域的高重组率造成的。研究发现,对于 TiO2/i-CsSnI3/p-CsSnI3、TiO2/i-CsGeI3/p-CsGeI3 和 TiO2/i-CsSn0.5Ge0.5I3/p-CsSn0.5Ge0.5I3,如果能有效控制高掺杂在 HTLs 中产生的缺陷,n-p 结构比传统的 ni-p 结构具有更好的光伏性能(i 膜厚度趋近于零)。PSCs 的效率对缺陷密度和缺陷水平位置非常敏感,缺陷密度对光伏性能的影响大于缺陷水平位置。当缺陷密度低于约 5 × 1017 cm-3 时,太阳能电池仍能保持较高的功率转换效率。此外,我们还发现界面陷阱密度的增加会降低 PSC 的光伏性能。我们的研究为基于 CsSnxGe1-xI3 的 PSCs 的优化设计提供了启示。
{"title":"Simulation Study on the All-Inorganic CsSnxGe1–xI3-Based Perovskite Solar Cells Using Isotypic Perovskites as Hole Transport Layers","authors":"Shuo Lin,&nbsp;Baoping Zhang,&nbsp;Weichao Wang,&nbsp;Tie-Yu Lü,&nbsp;Jinrong Zhou,&nbsp;Xiuyan Li,&nbsp;Yuhong Fang and Jin-Cheng Zheng*,&nbsp;","doi":"10.1021/acs.energyfuels.4c0396010.1021/acs.energyfuels.4c03960","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.4c03960https://doi.org/10.1021/acs.energyfuels.4c03960","url":null,"abstract":"<p >All-inorganic Sn–Ge-based perovskite solar cells (PSCs) have made great progress in recent years. Furthermore, they can be used as promising lead-free absorbers for PSCs, and <i>p</i>-type-doped CsSnI<sub>3</sub>, CsGeI<sub>3</sub>, and CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub> could also be used as good hole transport layers (HTLs). In this simulation work, CsSnI<sub>3</sub>, CsGeI<sub>3</sub>, and CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub> are used as both absorbers and HTLs. The effects of the dopant concentration of HTLs, the thickness of absorbers, and HTLs on the photovoltaic performance of PSCs were studied to optimize the device structures. The maximum efficiencies from high to low are 28.35%, 26.35%, 25.84%, 25.23%, 18.83%, 17.49%, and 11.79% for the TiO<sub>2</sub>/<i>i</i>-CsSnI<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub>/<i>p</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsSnI<sub>3</sub>/<i>p</i>-CsGeI<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub>/<i>p</i>-CsGeI<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsGeI<sub>3</sub>/<i>p</i>-CsGeI<sub>3</sub>, and TiO<sub>2</sub>/<i>i</i>-CsGeI<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub>, respectively. The TiO<sub>2</sub>/<i>i</i>-CsGeI<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub> cell exhibits the lowest efficiency of 11.79% in all of the simulated PSCs due to the spike-like band offset at the <i>i</i>-CsGeI<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub> interface and high recombination rate in the <i>p</i>-CsSnI<sub>3</sub> region. It is found that the <i>n</i>-<i>p</i> structures could have better photovoltaic performance (thickness of <i>i</i>-film approaching zero) than the conventional <i>n</i>-<i>i</i>-<i>p</i> structures for the TiO<sub>2</sub>/<i>i</i>-CsSnI<sub>3</sub>/<i>p</i>-CsSnI<sub>3</sub>, TiO<sub>2</sub>/<i>i</i>-CsGeI<sub>3</sub>/<i>p</i>-CsGeI<sub>3</sub>, and TiO<sub>2</sub>/<i>i</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub>/<i>p</i>-CsSn<sub>0.5</sub>Ge<sub>0.5</sub>I<sub>3</sub> PSCs if the defects in HTLs created by high doping can be effectively controlled. The efficiencies of PSCs are sensitive to the defect density and defect level position, and the influence of defect density on the PV performance is larger than that of the defect level position. The solar cells could maintain high power conversion efficiency for defect density below about 5 × 10<sup>17</sup> cm<sup>–3</sup>. Furthermore, the increase of the interface trap density is found to reduce the photovoltaic performance of PSCs. Our study provides insight into the optimal design of CsSn<sub><i>x</i></sub>Ge<sub>1–<i>x</i></sub>I<sub>3</sub>-based PSCs.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.2,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction to Effect of Ag Content on the Electrochemical Performance of Ag2Te Nanostructures Synthesized by Hydrothermal Route for Supercapacitor Applications 改正水热法合成的 Ag2Te 纳米结构的银含量对其在超级电容器应用中的电化学性能的影响
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-07 DOI: 10.1021/acs.energyfuels.4c0363510.1021/acs.energyfuels.4c03635
Muhammad Abdullah, Norah Alwadai, Maryam Al Huwayz, Sumaira Manzoor, Peter John*, Abdul Ghafoor Abid, Muhammad Ishfaq Ghouri, Salma Aman, Mohammaed Sultan Al-Buriahi and Muhammad Naeem Ashiq*, 
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引用次数: 0
Development of a Skeletal Mechanism with NOx Chemistry for CH4/H2 Combustion over a Wide Range of Hydrogen-Blending Ratios 在宽广的氢气混合比范围内,为 CH4/H2 燃烧开发氮氧化物化学骨架机制
IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-07 DOI: 10.1021/acs.energyfuels.4c0280210.1021/acs.energyfuels.4c02802
Shunta Xu, Ziyi Tian and Hao Liu*, 

An accurate and efficient skeletal mechanism is critical to describe the combustion chemistry of CH4/H2 with nitrogen oxides (NOx) through computational fluid dynamics (CFD) simulations. In this paper, the performance of the 11 classical/state-of-the-art detailed C/H/O/N mechanisms (1995–2020) for predicting combustion of CH4, H2, and their mixtures is comprehensively and quantitatively evaluated. Based on the best-performing one Glarborg2018, a 60-species and 566-reaction skeletal C1–2/H/O/N mechanism with NOx chemistry for CH4/H2 combustion over a wide range of hydrogen-blending ratios from 0 to 100% is developed using the directed relation graph with error propagation (DRGEP), sensitivity analysis (SA), and quasi-steady-state-approximation (QSSA) methods. Also, the present newly developed skeletal mechanism is comprehensively evaluated against large numbers of available experimental data (∼3500 data points) for combustion of CH4, H2, and their mixtures, in terms of ignition delay times, laminar burning velocities, flame structures (i.e., temperature and species (reactants, intermediates, and final products, including CH4, H2, O2, CO, CO2, CH2O, C2H4, C2H6, N2, and H2O) concentrations), NOx emissions, as well as NO formation and reduction via different submechanisms. Results show that Glarborg2018 performs best in predicting NO from combustion of CH4, H2, and their mixtures, especially at high temperatures. The present newly developed skeletal mechanism can reasonably well predict NOx emissions in CH4/H2 combustion over a wide range of hydrogen-blending ratios from 0 to 100% at low-/intermediate-/high-temperature levels (e.g., 650–2200 K), which is superior to the existing skeletal ones; in particular, thermal NO, prompt NO, NO formed via NNH and N2O-intermediate, as well as NO reduced by HCCO/CHi=0–3 and H can be separately reproduced. In conclusion, the present newly developed skeletal C1–2/H/O/N mechanism preserves comparable prediction accuracy compared to its parent Glarborg2018 and is applicable to model combustion of CH4, H2, and their mixtures with NOx chemistry over a wide range of low, intermediate, and high temperatures.

要通过计算流体动力学(CFD)模拟来描述 CH4/H2 与氮氧化物(NOx)的燃烧化学反应,准确高效的骨架机理至关重要。本文全面、定量地评估了 11 种经典/最先进的详细 C/H/O/N 机理(1995-2020 年)在预测 CH4、H2 及其混合物燃烧方面的性能。在性能最佳的 Glarborg2018 机理的基础上,利用有向关系图与误差传播(DRGEP)、灵敏度分析(SA)和准稳态近似(QSSA)方法,开发了一种 60 种、566 个反应的 C1-2/H/O/N 骨架机理,该机理具有氮氧化物化学性质,适用于氢气混合比从 0 到 100% 的宽范围内的 CH4/H2 燃烧。此外,还根据大量可用的实验数据(∼3500 个数据点),从点火延迟时间、层流燃烧速度、火焰结构(即:温度和物种(反应物、中间产物和反应物))等方面,对目前新开发的骨架机理进行了全面评估、温度和物种(反应物、中间产物和最终产物,包括 CH4、H2、O2、CO、CO2、CH2O、C2H4、C2H6、N2 和 H2O)浓度)、氮氧化物排放以及通过不同子机制形成和还原氮氧化物。结果表明,Glarborg2018 在预测 CH4、H2 及其混合物燃烧产生的 NO 方面表现最佳,尤其是在高温条件下。新开发的骨架机理可以在低温/中温/高温(如 650-2200 K)条件下,在 0 到 100% 的氢气混合比范围内合理预测 CH4/H2 燃烧中的氮氧化物排放,优于现有的骨架机理;特别是可以分别再现热氮氧化物、瞬时氮氧化物、通过 NNH 和 N2O-中间产物形成的氮氧化物,以及通过 HCCO/CHi=0-3 和 H 还原的氮氧化物。总之,目前新开发的 C1-2/H/O/N 骨架机理与其母体 Glarborg2018 相比,保持了相当高的预测精度,并适用于 CH4、H2 及其混合物在低、中、高温范围内与 NOx 化学反应的模型燃烧。
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