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Improved nickel nanocatalysts for selective cleavage of lignin model compounds and lignin 用于选择性裂解木质素模型化合物和木质素的改良型纳米镍催化剂
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-28 DOI: 10.1016/j.biombioe.2024.107186
Hao Zhao , Chongbo Cheng , Benkai Zhu , Youzhi Yang , Qichang Wang , Dekui Shen , Xiaoxiang Jiang

The selective hydrogenolysis of lignin offers a promising avenue for converting lignin into valuable chemicals and fuels. However, the development of highly active catalysts for this process remains challenging. In this study, a series of Nix/Al2O3 catalysts were synthesized by calcining and reducing layered double hydroxides (LDHs) precursors. These catalysts were evaluated for their effectiveness in catalyzing the conversion of lignin-derived model compounds (2-phenoxy-1-phenylethanol and diphenyl ether). Remarkably, the optimized Ni3/Al2O3 catalyst demonstrated exceptional performance in cleaving C–O bonds, achieving complete conversion with high selectivity for monomers product under reaction conditions of 200 °C, 1 MPa H2, and 1 h. The catalyst's outstanding performance can be attributed to its relatively large specific surface area, Ni loading exceeding 50 wt%, well-dispersed Ni metal particles, abundant surface oxygen vacancies, and a significant number of acid sites. Additionally, the hydrogenolysis of lignin using the Ni3/Al2O3 catalyst resulted in a substantial production of monophenols (15.0 wt%). This study introduces a novel approach for tailoring highly active Ni nanocatalysts and highlights the capability of Nix/Al2O3 catalysts to efficiently cleave C–O bonds in lignin under mild reaction conditions.

木质素的选择性氢解为将木质素转化为有价值的化学品和燃料提供了一条前景广阔的途径。然而,为这一过程开发高活性催化剂仍具有挑战性。本研究通过煅烧和还原层状双氢氧化物(LDHs)前驱体合成了一系列 Nix/Al2O3 催化剂。对这些催化剂催化木质素衍生模型化合物(2-苯氧基-1-苯乙醇和二苯醚)转化的有效性进行了评估。催化剂的优异性能归功于其相对较大的比表面积、超过 50 wt% 的镍负载量、分散良好的镍金属颗粒、丰富的表面氧空位以及大量的酸位点。此外,使用 Ni3/Al2O3 催化剂对木质素进行氢解,可产生大量单酚(15.0 wt%)。本研究介绍了一种定制高活性镍纳米催化剂的新方法,并强调了 Nix/Al2O3 催化剂在温和的反应条件下高效裂解木质素中 C-O 键的能力。
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引用次数: 0
Sn-modified SBA-15 with tailored acid properties for efficient 5-hydroxymethylfurfural production from glucose 具有定制酸特性的锡改性 SBA-15 可从葡萄糖中高效生产 5-羟甲基糠醛
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-28 DOI: 10.1016/j.biombioe.2024.107202
Mengjiao Yu, Xiong-Fei Zhang, Yunhua Bai, Lian Shu, Jianfeng Yao

Interest in production and utilization of 5-hydroxymethylfurfural (5-HMF) has risen greatly as 5-HMF is considered as an extremely important platform compound. It remains a huge challenge to develop efficient and low-cost solid catalysts with suitable acid properties for sustainable production of 5-HMF from glucose. Herein, a bifunctional Sn-modified SBA-15 (Sn–OH/SBA-15) catalyst containing both Lewis and Brønsted acid sites was fabricated. Dimethyldichlorostannane was grafted onto mesoporous SBA-15, and the methyl groups were then converted to hydroxyl groups by calcination. The synergistic effects of Lewis and Brønsted acid significantly boosted the synthesis of 5-HMF from glucose adopting the one-pot method. By optimizing the reaction conditions, the Sn–OH/SBA-15 sample was able to achieve a glucose conversion of 96.9% with a 5-HMF yield of 70.6% (180 °C, 5 h). Moreover, the catalyst demonstrated superior recyclability and reusability. This work would enlighten the exploitation and preparation of highly efficient catalysts for the transformation of carbohydrates into value-added chemicals.

5-hydroxymethylfurfural (5-HMF) 被认为是一种极其重要的平台化合物,因此人们对 5-hydroxymethylfurfural (5-HMF) 的生产和利用兴趣大增。为从葡萄糖中持续生产 5-HMF 开发具有合适酸性的高效、低成本固体催化剂仍然是一项巨大的挑战。在此,我们制备了一种双功能 Sn 改性 SBA-15 (Sn-OH/SBA-15)催化剂,该催化剂同时含有路易斯酸位点和布氏酸位点。将二甲基二氯锡烷接枝到介孔 SBA-15 上,然后通过煅烧将甲基转化为羟基。路易斯酸和布伦司特酸的协同作用大大提高了采用一锅法从葡萄糖合成 5-HMF 的效率。通过优化反应条件,Sn-OH/SBA-15 样品的葡萄糖转化率达到 96.9%,5-HMF 收率达到 70.6%(180 °C,5 小时)。此外,该催化剂还具有优异的可回收性和可再利用性。这项工作将有助于开发和制备将碳水化合物转化为高附加值化学品的高效催化剂。
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引用次数: 0
Enzymolytic lignin derived Fe–N codoped porous carbon materials as catalysts for oxygen reduction reactions 作为氧还原反应催化剂的酶解木质素衍生 Fe-N 共掺多孔碳材料
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-27 DOI: 10.1016/j.biombioe.2024.107173
Xia Qu , Yantao Yang , Lili Dong , Zheng Li , Yuwei Feng , Tingzhou Lei , Suxia Ren

Numerous active sites and hierarchical pore structures are important for improving catalytic performance for the oxygen reduction reaction (ORR). In this work, a series of iron-nitrogen-doped porous carbon materials (Fe–N–C) with ORR catalytic activity were prepared by a one-step pyrolysis method using enzymolytic lignin as the raw material, soy protein isolate and iron chloride as dopants. The results showed that the samples with the best performance have abundant Fe-Nx active sites and mesoporous structures. At the same time, the electrocatalytic results indicate that the half-wave potential of catalyst was 0.84 V, which reached 96.55% of commercial Pt/C catalysts (E1/2 = 0.86 V), it still preserves an initial current density of 92%, after 10,000 s of circulation, which is much better than Pt/C (86%). Due to the low cost, high activity and stable ORR property, the prepared non-precious metal electrocatalyst will play an important role in the applications of fuel cells.

大量的活性位点和分层孔隙结构对于提高氧还原反应(ORR)的催化性能非常重要。本研究以酶解木质素为原料,以大豆分离蛋白和氯化铁为掺杂剂,通过一步热解法制备了一系列具有 ORR 催化活性的铁氮掺杂多孔碳材料(Fe-N-C)。结果表明,性能最好的样品具有丰富的 Fe-Nx 活性位点和介孔结构。同时,电催化结果表明,催化剂的半波电位为 0.84 V,达到商用 Pt/C 催化剂(E1/2 = 0.86 V)的 96.55%,循环 10000 s 后仍能保持 92% 的初始电流密度,远优于 Pt/C(86%)。由于制备的非贵金属电催化剂具有低成本、高活性和稳定的 ORR 特性,它将在燃料电池的应用中发挥重要作用。
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引用次数: 0
Influence of reaction parameters on biofuels derived from solvothermal liquefaction of Citrus limetta fruit wastes 反应参数对柑橘类水果废料溶热液化产生的生物燃料的影响
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-27 DOI: 10.1016/j.biombioe.2024.107183
Sneha Acharya, Nanda Kishore

Citrus limetta or sweet lime is a widely consumed fruit worldwide. The wastes generated from their processing are enormous and are discarded without any value-addition. Biomass liquefaction in hydrogen-donor solvent is an effective thermochemical conversion technique to produce value added products such as biocrude and biochar from wet biomasses directly. Thus, liquefaction studies of Citrus limetta peel and pulp were conducted using solvent methanol at temperatures of 240 °C–280 °C, 30 min residence time as well as 1:2, 1:3 and 1:4 ratios of biomass to solvent. The impact of temperature as well as biomass to solvent ratio on yield of biocrude and biochar were investigated herein. Biocrude produced from Citrus limetta peel at 240 °C and 1:3 ratio of biomass to solvent is maximum (12.5 wt. %). At reaction parameters of 280 °C and 1:4 ratio of biomass to solvent, biocrude from Citrus limetta pulp showed higher heating value of 27.18 MJ kg−1 which was the maximum obtained in this study. The gas-chromatography mass-spectrometry (GC-MS) indicated presence of alcohols, phenols, alkanes, ketones, ethers, esters and fatty acid methyl esters as major compounds. The characteristics and energy content of biochar demonstrated their potentiality for bioenergy applications.

柑橘或甜酸橙是全世界广泛食用的水果。其加工过程中产生的废弃物数量巨大,而且没有任何附加值就被丢弃。生物质在供氢溶剂中液化是一种有效的热化学转化技术,可直接从湿生物质中生产生物原油和生物炭等增值产品。因此,在 240 ℃-280 ℃、30 分钟停留时间以及生物质与溶剂比例为 1:2、1:3 和 1:4 的条件下,使用甲醇溶剂对柠檬果皮和果肉进行了液化研究。本文研究了温度以及生物质与溶剂比例对生物原油和生物炭产量的影响。在 240 °C、生物质与溶剂比例为 1:3 的条件下,柑橘类果皮产生的生物原油最多(12.5 wt.%)。在 280 °C、生物质与溶剂比例为 1:4 的反应参数下,从柠檬果肉中提取的生物原油显示出较高的热值,达到 27.18 兆焦耳/千克-1,这是本研究中获得的最大值。气相色谱-质谱联用仪(GC-MS)显示,主要化合物有醇、酚、烷、酮、醚、酯和脂肪酸甲酯。生物炭的特性和能量含量显示了其在生物能源应用方面的潜力。
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引用次数: 0
Application of optical diagnosis technology in biomass combustion 生物质燃烧中光学诊断技术的应用
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-27 DOI: 10.1016/j.biombioe.2024.107198
Beibei Yan , Jingwen Lv , Shengquan Zhou , Zhaoting Wu , Xiaoyun Liu , Bo Li , Qiang Gao , Wenzhu Wu , Guanyi Chen

Biomass is the only carbon-neutral fuel, the development and utilization of biomass are crucial for achieving carbon neutrality. However, the combustion of biomass in boilers is often unstable due to the heterogeneity of biomass raw materials, leading to a decrease in combustion efficiency and an increase in pollutant emissions. Continuous online monitoring is essential for the safe, stable and efficient operation of boilers. Traditional measurement methods typically rely off-line analysis to study the kinetics of biomass oxidation and pyrolysis. These methods struggle to accurately capture transient parameters during combustion due to changes in reaction pathways and oxidant products. Optical diagnosis is a non-contact, instantaneous and efficient method that can achieve in-situ, online and rapid measurement of multiple parameters. This technology has been extensively applied by researchers in the field of biomass combustion diagnosis. The current status and applications of online measurement methods for biomass ignition/combustion behavior and soot generation are reviewed. The problems and development trends of existing optical diagnostic technologies for biomass combustion are also been proposed. The review suggests that the future development of more diverse and effective optical diagnostic techniques, as well as the combination of various diagnostic technologies, is beneficial for comprehensively analyzing the key issues in biomass combustion, so as to realize the efficient utilization of biomass.

生物质是唯一的碳中和燃料,开发和利用生物质对实现碳中和至关重要。然而,由于生物质原料的异质性,生物质在锅炉中的燃烧往往不稳定,导致燃烧效率降低和污染物排放增加。持续在线监测对于锅炉的安全、稳定和高效运行至关重要。传统的测量方法通常依靠离线分析来研究生物质氧化和热解的动力学。由于反应途径和氧化产物的变化,这些方法难以准确捕捉燃烧过程中的瞬态参数。光学诊断是一种非接触、瞬时和高效的方法,可实现多种参数的原位、在线和快速测量。这项技术已被研究人员广泛应用于生物质燃烧诊断领域。本文综述了生物质点火/燃烧行为和烟尘生成在线测量方法的现状和应用。还提出了现有生物质燃烧光学诊断技术存在的问题和发展趋势。综述认为,未来发展更多样、更有效的光学诊断技术,并将各种诊断技术相结合,有利于全面分析生物质燃烧的关键问题,从而实现生物质的高效利用。
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引用次数: 0
A hybrid approach of anaerobic digestion model no. 1 and machine learning to model and optimize continuous anaerobic digestion processes 厌氧消化模型 No.1 号厌氧消化模型与机器学习的混合方法,用于连续厌氧消化工艺的建模和优化
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-26 DOI: 10.1016/j.biombioe.2024.107176
Yadong Ge , Junyu Tao , Zhi Wang , Lan Mu , Wei Guo , Zhanjun Cheng , Beibei Yan , Yan Shi , Hong Su , Guanyi Chen

Anaerobic digestion is a promising approach to dispose of biodegradable waste and wastewater, generating biogas as an alternative energy resource. This work proposed a so-called M-CADM1 for continuous anaerobic digestion simulation, which combined the machine learning and anaerobic digestion model No.1 (ADM1). The detailed reaction path and intermediate products in different stages of anaerobic digestion are specified in ADM1. The kinetic parameters were modified by machine learning. The characteristics (elemental composition) of feedstocks were used to predict kinetic parameters. A total of 75 biomass samples were used to establish for machine learning models. Five element contents (C, H, O, N, S), feedstock feed rate, and anaerobic digestion temperature were used as the input. The kinetic parameters were set as output. The sensitivities of 17 kinetic parameters were evaluated. 7 kinetic parameters with the highest sensitivities were selected as ADM1 model inputs by sensitivity analysis. The R2 and RMSE were used as the index to evaluated the accuracy of machine learning model. The best R2 and RMSE reached 0.84 and 0.196. The TIC was used as the index to evaluated the accuracy of M-CADM1. By comparing the simulated value with the experimental value, the accuracy of the overall M-CADM1 expressed by TIC of kitchen waste was 0.036. The organic acid content and pH in the reactor were considered as indicators to study the accuracy and stability of the M-CADM1. Trends in organic acids, free ammonia or hydrogen inhibition, and pH were consistent with experimental continuous anaerobic digestion results.

厌氧消化是一种处理可生物降解废物和废水、产生沼气作为替代能源的有效方法。本研究提出了一种用于连续厌氧消化模拟的 M-CADM1,它将机器学习与厌氧消化模型 1 号(ADM1)相结合。厌氧消化模型 1 中规定了厌氧消化不同阶段的详细反应路径和中间产物。通过机器学习修改了动力学参数。原料的特征(元素组成)用于预测动力学参数。机器学习模型共使用了 75 个生物质样本。五种元素含量(C、H、O、N、S)、原料进料速度和厌氧消化温度被用作输入。动力学参数被设定为输出。对 17 个动力学参数的敏感性进行了评估。通过灵敏度分析,选择了 7 个灵敏度最高的动力学参数作为 ADM1 模型的输入。用 R2 和 RMSE 作为评价机器学习模型准确性的指标。最佳 R2 和 RMSE 分别为 0.84 和 0.196。TIC 被用作评估 M-CADM1 精度的指标。通过比较模拟值和实验值,用厨余 TIC 表示的 M-CADM1 整体准确度为 0.036。反应器中的有机酸含量和 pH 值被视为研究 M-CADM1 精确度和稳定性的指标。有机酸、游离氨或氢抑制以及 pH 值的变化趋势与连续厌氧消化实验结果一致。
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引用次数: 0
A review of breakthroughs in biodiesel production with transition and non-transition metal-doped CaO nano-catalysts 使用过渡金属和非过渡金属掺杂的 CaO 纳米催化剂生产生物柴油的突破性进展综述
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-26 DOI: 10.1016/j.biombioe.2024.107158
Rabiah Amal , Muhammad Usman

The rising energy demand, coupled with increasing pollution and the depletion of fossil fuel reserves, has led to an urgent need for sustainable fuel alternatives like biodiesel. However, biodiesel production is not without its challenges, especially when using homogeneous catalysis, which often results in soap formation and high wastewater production. This review focuses on the use of heterogeneous base catalysts, particularly calcium oxide (CaO) doped with transition and non-transition metals, as a more efficient method for biodiesel production from various raw materials. The inclusion of transition and non-transition metal dopants in CaO catalysts plays a crucial role in enhancing their performance. These dopants significantly increase the surface area of the catalysts, leading to higher biodiesel yields (84.9–99.7%) and offering a marked improvement over traditional homogeneous catalysis methods. The study delves into the reaction mechanisms, thermodynamics, comparison of economic aspects of using heterogeneous and homogeneous catalysts, life cycle assessment (LCA), and practical implications of this study. It highlights that metal-doped heterogeneous catalysts are not only more efficient but also offer environmental benefits such as the emission of fewer pollutants and cost benefits due to reusability, ease of separation, and cheaper maintenance. In addition, future research should explore the untapped potential of new dopants and waste materials for developing cost-effective and sustainable catalysts. Investigating statistical methods and optimization models is crucial for finding optimal conditions for efficient biodiesel production.

能源需求不断增长,加上污染日益严重和化石燃料储备日渐枯竭,人们迫切需要生物柴油等可持续燃料替代品。然而,生物柴油的生产并非没有挑战,尤其是在使用均相催化剂时,往往会导致肥皂的形成和大量废水的产生。本综述重点介绍使用异相基催化剂,特别是掺杂过渡金属和非过渡金属的氧化钙(CaO),作为利用各种原料生产生物柴油的更有效方法。在 CaO 催化剂中加入过渡金属和非过渡金属掺杂剂对提高其性能起着至关重要的作用。这些掺杂剂大大增加了催化剂的表面积,从而提高了生物柴油的产量(84.9-99.7%),与传统的均相催化方法相比有了明显的改进。本研究深入探讨了反应机理、热力学、使用异相催化剂和均相催化剂的经济性比较、生命周期评估(LCA)以及本研究的实际意义。研究强调,掺杂金属的异质催化剂不仅效率更高,还具有环境效益,如污染物排放量更少,以及可重复使用、易于分离和维护成本更低等成本优势。此外,未来的研究应探索新掺杂剂和废料的未开发潜力,以开发具有成本效益和可持续发展的催化剂。研究统计方法和优化模型对于找到高效生产生物柴油的最佳条件至关重要。
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引用次数: 0
Culture of photosynthetic microalgae consortium in artificial produced water supplemented with liquid digestate in closed column photobioreactors and open-pond raceway 在封闭式柱状光生物反应器和开放式池塘赛道中,用人工生产的水和液态沼渣培养光合微藻群
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-25 DOI: 10.1016/j.biombioe.2024.107165
Aurélien Parsy , Elena Ficara , Valeria Mezzanotte , Marco Mantovani , Rémy Guyoneaud , Florian Monlau , Cecilia Sambusiti

Large amounts of produced water are extracted by the Oil and Gas energy sector since the industrial revolution. This available water, often salty, can be used to dilute liquid digestate from the anaerobic digestion process, a promising source of nutrients for microalgae cultivation. The study investigates the growth of halotolerant microalgae and their associated bacteria in column photobioreactors (PBRs) and open raceway pond (RWP), to treat industrial wastewaters while producing biomass for energy valorisation. Microalgae were cultured in mixtures of saline artificial produced water (7–44 %v/v), liquid digestate (5 %v/v using PBRs, 29–63 %v/v using RWP) and seawater. Nannochloropsis oceanica and Tetraselmis suecica strains were firstly cultivated in 70 L PBRs in indoor conditions for 3 months and later in 1.1 m3 RWP operated in outdoor conditions for 5 months in spring-summer period. In PBRs, average productivity was 9.0 ± 4.2 gVSS·m−2·d−1 (102–153 mgVSS·L−1·d−1), with daily removal efficiencies for chemical oxygen demand, nitrogen and phosphorous up to 61.8, 31.6 and 97.2 %, respectively. In RWP, strong changes in the microalgae populations were observed. Productivity was 6.7 ± 5.2 gVSS·m−2·d−1 (30 ± 23 mgVSS·L−1·d−1), with daily removal efficiencies for chemical oxygen demand, nitrogen and phosphorous up to 48.4, 44.4 and 88.1 %, respectively. In parallel with the production of microalgae, a nitrifying microbial population grew in the RWP despite the high salinity (70 g L−1). Over these periods of several months, microalgae production was maintained using a culture medium containing high salt concentration, metals and harmful aromatic compounds.

自工业革命以来,石油和天然气能源行业提取了大量的采出水。这些可利用的水通常含盐,可用于稀释厌氧消化过程中产生的液态沼渣,这是微藻类培养很有前景的营养来源。本研究调查了耐盐微藻及其相关细菌在柱式光生物反应器(PBR)和开放式赛道池塘(RWP)中的生长情况,以处理工业废水,同时生产生物质,实现能源价值化。微藻类在含盐人工生产用水(7-44 %v/v)、液态沼渣(使用 PBRs 时为 5 %v/v,使用 RWP 时为 29-63 %v/v)和海水的混合物中进行培养。在春夏季节,首先在室内 70 升 PBR 中培养海洋藻类(Nannochloropsis oceanica)和四鳃藻(Tetraselmis suecica)3 个月,然后在室外 1.1 立方米 RWP 中培养 5 个月。在 PBR 中,平均生产率为 9.0 ± 4.2 gVSS-m-2-d-1 (102-153 mgVSS-L-1-d-1),化学需氧量、氮和磷的日去除率分别达到 61.8%、31.6% 和 97.2%。在 RWP 中,观察到微藻种群发生了很大变化。产量为 6.7 ± 5.2 gVSS-m-2-d-1(30 ± 23 mgVSS-L-1-d-1),化学需氧量、氮和磷的日去除率分别达到 48.4%、44.4% 和 88.1%。在产生微藻的同时,尽管盐度很高(70 g L-1),RWP 中的硝化微生物种群也在增长。在这几个月的时间里,微藻类的生产一直使用含有高浓度盐、金属和有害芳香族化合物的培养基。
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引用次数: 0
Engineering biochar-supported nickel catalysts for efficient CO2 methanation 工程生物炭支撑镍催化剂用于高效 CO2 甲烷化
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-25 DOI: 10.1016/j.biombioe.2024.107179
Alexandra J. Frainetti , Naomi B. Klinghoffer

Carbon dioxide methanation is a promising approach to convert captured CO2 into green natural gas. Developing high performance biochar-supported nickel catalysts promotes a circular economy and the application of sustainable catalysts. Western red cedar biochar was produced via pyrolysis at 400, 500, and 600 °C and loaded with nickel via incipient wetness impregnation. Methanation was done at 400, 500, and 600 °C with the highest methane yield of 59% achieved at 500 °C with 10 wt.% Ni loading. This is comparable to a γ-Al2O3 supported catalyst prepared and tested similarly, which achieved a methane yield of 53%. Biochar-supported catalysts showed deactivation whereby methane yield decreased from 59% to 51% over 5 h, likely due to coking and/or the sintering of nickel. Various space velocities were tested, and results demonstrated that with a space velocity of 37.5 mL/g.min methane selectivity was 89% after 1 h on stream compared to methane selectivity of 42%, which was achieved at a space velocity of 112.5 mL/g.min. This shows that a much higher rate of deactivation is observed at higher space velocities. Increasing the nickel loading from 5 wt.% to 10 wt.% increased methane yield from 40% to 58% after 1 h on stream. The higher loading also showed significantly less deactivation. Future work focusing on the extent and impact of metal-support interactions and metal dispersion on catalytic performance and deactivation during CO2 methanation is recommended.

二氧化碳甲烷化是将捕获的二氧化碳转化为绿色天然气的一种前景广阔的方法。开发高性能生物炭支撑镍催化剂可促进循环经济和可持续催化剂的应用。西部红柏生物炭是在 400、500 和 600 °C 高温下热解产生的,并通过初湿浸渍法添加了镍。甲烷化在 400、500 和 600 °C 温度下进行,在 500 °C 温度下甲烷产量最高,达到 59%,镍负载量为 10 wt.%。这与类似制备和测试的 γ-Al2O3 支持催化剂相当,后者的甲烷产率为 53%。生物炭支撑的催化剂出现了失活现象,甲烷产量在 5 小时内从 59% 降至 51%,这可能是由于结焦和/或镍烧结造成的。对各种空间速度进行了测试,结果表明,在 37.5 毫升/克.分的空间速度下,甲烷的选择性在运行 1 小时后达到 89%,而在 112.5 毫升/克.分的空间速度下,甲烷的选择性仅为 42%。这表明,空间速度越高,失活率越高。将镍的负载量从 5 wt.% 提高到 10 wt.%,甲烷的产量在运行 1 小时后从 40% 提高到 58%。较高的装载量也明显减少了失活现象。建议今后重点研究金属-支撑相互作用和金属分散对二氧化碳甲烷化过程中催化性能和失活的程度和影响。
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引用次数: 0
Utilization of waste tea leaves as metal-free catalyst for hydrogen generation via ethanolysis of Sodium Borohydride 利用废茶叶作为无金属催化剂,通过乙醇分解硼氢化钠制氢
IF 6 2区 生物学 Q1 Agricultural and Biological Sciences Pub Date : 2024-03-23 DOI: 10.1016/j.biombioe.2024.107168
Naman Srivastava , Madhu Agarwal , Neha Pal , Rajeev Kumar Dohare

In the present study, waste green and black tea leaves have been used to synthesize metal–free catalysts for hydrogen generation by ethanolysis of sodium borohydride by the acetic acid activation and carbonization. The FTIR, BET, SEM-EDS, and XPS characterizations have been performed to analyze the synthesized catalysts' properties. The parameters such as amounts of catalysts, SB, and reaction temperature were studied while performing the experiments. They were optimized using the Response Surface Methodology (RSM) to obtain the highest values of Hydrogen Generation Rates (HGR) of 1350 ml min−1 g catalyst−1 and 2700 ml min−1 g catalyst−1 using the acetic acid activated black tea (AA – BT) and acetic acid activated green tea (AA – GT) catalysts respectively with the activation energies of 13.14 kJ mol−1 and 37 kJ mol−1. The BET analysis has revealed that the AA – GT and AA – BT catalysts have surface areas of 22.96 m2 g−1 and 3.28 m2 g−1, pore diameters of 1.72 nm and 1.70 nm and pore volumes of 0.0047 and 0.0331785 m3 g−1 respectively. The electrochemical analysis has revealed that the synthesized metal–free catalysts AA – BT and AA - GT possess good specific capacitances of 63.77 mF cm−2 and 121 mF cm−2, which shows that both can be used as electrode material for energy storage applications. Hence, it can be believed that both metal–free catalysts can act as dual functional materials, which can act as catalysts and energy storage materials.

本研究利用废弃的绿茶叶和红茶叶,通过乙酸活化和碳化,合成了无金属催化剂,用于硼氢化钠的乙醇分解制氢。傅立叶变换红外光谱、BET、SEM-EDS 和 XPS 表征分析了合成催化剂的特性。在进行实验时,对催化剂用量、SB 和反应温度等参数进行了研究。使用响应面方法(RSM)对这些参数进行了优化,结果发现,使用醋酸活化红茶(AA - BT)和醋酸活化绿茶(AA - GT)催化剂,氢气生成率(HGR)分别为 1350 毫升/分钟-1 克催化剂-1 和 2700 毫升/分钟-1 克催化剂-1,活化能分别为 13.14 kJ mol-1 和 37 kJ mol-1。BET 分析显示,AA - GT 和 AA - BT 催化剂的表面积分别为 22.96 m2 g-1 和 3.28 m2 g-1,孔径分别为 1.72 nm 和 1.70 nm,孔体积分别为 0.0047 和 0.0331785 m3 g-1。电化学分析表明,合成的无金属催化剂 AA - BT 和 AA - GT 具有良好的比电容,分别为 63.77 mF cm-2 和 121 mF cm-2,这表明它们都可用作储能应用的电极材料。因此,可以认为这两种无金属催化剂都可以作为双功能材料,既可以作为催化剂,也可以作为储能材料。
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Biomass & Bioenergy
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