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Recent advances in the catalytic production of bio-based diol 2,5-bis(hydroxymethyl)furan 催化制备生物基二醇2,5-双(羟甲基)呋喃的研究进展
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2023.01.001
Wenguang Zhao , Feng Wang , Kangyu Zhao , Xianxiang Liu , Xiaoting Zhu , Le Yan , Yuan Yin , Qiong Xu , Dulin Yin

Biomass-derived 2,5-bis(hydroxymethyl)furan (BHMF) has received great attention and interest due to its broad application prospects in polyesters and medicine. Over the past decades, the catalytic systems including thermocatalytic, biocatalytic, electrocatalytic, and photocatalytic hydrogenation of 5-hydroxymethylfurfural (HMF) into BHMF have been developed to a great extent. To understand the present status and challenges of BHMF production, this review systematically evaluates recent findings and developments of HMF hydrogenation through various reaction systems, with an emphasis on catalyst screening, synthesis processes, and reaction mechanism. Furthermore, a few potential research trends are also proposed, in order to provide innovative ideas for further exploration of BHMF synthesis in a simpler, efficient, and economical way.

生物质衍生的2,5-双(羟甲基)呋喃(BHMF)因其在聚酯和医药领域的广泛应用前景而备受关注和关注。近几十年来,5-羟甲基糠醛(HMF)加氢成BHMF的热催化、生物催化、电催化、光催化等催化体系得到了很大发展。为了了解甲基糠醛生产的现状和挑战,本文系统地评价了各种反应体系中甲基糠醛加氢的最新发现和进展,重点介绍了催化剂筛选、合成工艺和反应机理。此外,本文还提出了一些潜在的研究趋势,以期为进一步探索更简单、高效、经济的BHMF合成方法提供创新思路。
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引用次数: 2
Removal of Cr(VI) from aqueous solution by Rice-husk-based activated carbon prepared by Dual-mode heating method 双模加热法制备稻壳基活性炭去除水溶液中的铬(VI
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2023.01.003
Xinchi Zhang, Shiliang Wu, Yuan Liu, Ziwei Wang, Huiyan Zhang, Rui Xiao

Rice husk-based activated carbon was prepared with the help of zinc chloride using microwave and electrical dual-mode heating. The pore characteristics and chemical properties of rice husk-based activated carbon (RH-AC) were characterized by BET, XRD, Raman spectra, FTIR and pHIEP (pH of isoelectric point). The specific surface area of RH-AC is 1719.32 m2/g with a total pore volume of 1.05 cm3/g. The performance of RH-AC for removing Cr(VI) from aqueous solution was examined considering the variation of the contact time (0–120 min), pH value (2.0–9.0), adsorbent dose (0.5–3.0 g/L), initial concentration (28–145 mg/L) and solvent temperature (15–45 °C). The ideal pH for Cr(VI) removal is between 2.0 and 3.0 with the equilibrium time of 90 min, achieving the maximum adsorption capacity of 56.82 mg/g with the pH of 3.0. Comparable study on the established kinetic models and isotherms to simulate the removal of Cr(VI) by RH-AC was carried out to sort out the inherent mechanism of the absorption. Reasonable agreements could be obtained by the pseudo-second-order kinetic model and Langmuir, Freundlich and Tempkin isothermal models. Results from Body model simulation suggest that external mass transfer was the essential cause for rate-controlling in the adsorption process of Cr(VI).

以氯化锌为原料,采用微波和电双模加热法制备稻壳基活性炭。采用BET、XRD、拉曼光谱、FTIR和等电点pH对稻壳基活性炭(RH-AC)的孔隙特征和化学性质进行了表征。RH-AC的比表面积为1719.32 m2/g,总孔容为1.05 cm3/g。考察了RH-AC在接触时间(0 ~ 120 min)、pH值(2.0 ~ 9.0)、吸附剂剂量(0.5 ~ 3.0 g/L)、初始浓度(28 ~ 145 mg/L)、溶剂温度(15 ~ 45℃)等条件下去除水溶液中Cr(VI)的性能。吸附Cr(VI)的理想pH为2.0 ~ 3.0,平衡时间为90 min,当pH为3.0时吸附量最大,为56.82 mg/g。对建立的动力学模型和等温线进行对比研究,模拟RH-AC对Cr(VI)的吸附,以梳理吸附的内在机理。拟二级动力学模型与Langmuir、Freundlich和Tempkin等温模型吻合较好。体模型模拟结果表明,外传质是Cr(VI)吸附过程中速率控制的重要原因。
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引用次数: 1
Application of ionic liquids in CO2 capture and electrochemical reduction: A review 离子液体在CO2捕集和电化学还原中的应用综述
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2023.02.003
Xiaowei An , Peifen Wang , Xuli Ma , Xiao Du , Xiaogang Hao , Ziyuan Yang , Guoqing Guan

As a new type of green solvent with non-volatility, high thermal stability, high conductivity and various adjustable properties, ionic liquid (IL) has been widely used in the capture and electrochemical reduction of carbon dioxide (CO2). To date, many studies have been made to investigate CO2 capture by using different types of ILs and CO2 electrochemical reduction (CO2ER) with ILs as either electrolyte or other catalytic active components. Some structure–activity relationships between the structure and adsorption or catalytic properties of ILs have been found. Herein, the absorption performances and mechanisms of conventional ILs, amino-functionalized ILs, non-amino functionalized ILs and supported ILs for CO2 capture, as well as the performances and action mechanisms of ILs as the electrolyte, electrolyte additive, and/or electrode modifier in the process of CO2ER are summarized. Many researches indicate that the unique interaction between the anion or cation of IL and CO2 has a significant contribution to promote the absorption and conversion of CO2. However, the ILs used for CO2 capture and electrochemical reduction should be further explored. Especially, a more in-depth investigation of the adsorption and catalytic mechanisms with the help of quantum chemical calculation, molecular simulation, and in situ characterization techniques is necessary. It is expected to design and develop more efficient ILs used for CO2 capture and conversion on a large scale.

离子液体作为一种无挥发性、高热稳定性、高电导率和多种可调性质的新型绿色溶剂,在二氧化碳的捕获和电化学还原中得到了广泛的应用。迄今为止,已有许多研究通过使用不同类型的il和以il作为电解质或其他催化活性成分的CO2电化学还原(CO2ER)来研究CO2捕获。已经发现了il的结构与吸附或催化性能之间存在一定的构效关系。本文综述了传统液化油、氨基功能化液化油、非氨基功能化液化油和负载型液化油在CO2捕集中的吸收性能和机理,以及液化油作为CO2ER过程中的电解质、电解质添加剂和/或电极改性剂的性能和作用机理。许多研究表明,IL的阴离子或阳离子与CO2的独特相互作用对促进CO2的吸收和转化有重要贡献。然而,用于CO2捕集和电化学还原的il还有待进一步探索。特别是,有必要借助量子化学计算、分子模拟和原位表征技术对吸附和催化机理进行更深入的研究。预计将设计和开发用于大规模捕获和转换二氧化碳的更有效的ILs。
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引用次数: 7
Establishment of correlation between reaction kinetics and carbon structures in the char gasification process 煤焦气化反应动力学与碳结构相关性的建立
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2023.02.002
Zefeng Ge , Xi Cao , Zhenting Zha , Yuna Ma , Mingxun Zeng , Yuqing Wu , Zenghui Hou , Huiyan Zhang

For a gasification process, the char-CO2 gasification is the controlling step worthwhile to be deeply investigated. The article chosen corn stalk (CS), poplar sawdust (PS) and bagasse residue (BR) as the typical waste species derived from agricultural, forestal and industrial sources. The char-CO2 gasification behavior, reaction kinetics and carbon structure were studied to reveal the intrinsic factors determining the reaction kinetics. Generally, the carbon conversion and maximum conversion rate were influenced by the feedstocks species and char preparation temperatures, as influenced by ash proportion, potassium content in ash and carbon structure of char. The char-CO2 reaction for CS was subject more to the catalytic effect of alkali compositions, while pore structure affected more the gasification reaction for PS char. The isoconversional kinetic analysis indicated that the gasification reaction became stable at carbon conversion of 0.5. Subsequently, sectionalized kinetic parameters were calculated for the initial gasification temperature to the temperature reaching 50% conversion. The result showed that high initial gasification temperature increased the char-CO2 gasification barrier to hardly start the reaction but accelerate the reaction rate. The carbon structure analyses further clarified that the reaction activation energy was highly related to the microcrystalline structure of carbon, while the reaction rate was more determined by carbon pore structure.

对于一个气化过程,炭- co2气化是值得深入研究的控制步骤。本文选取玉米秸秆(CS)、杨木锯末(PS)和甘蔗渣(BR)作为典型的农业、林业和工业废弃物。通过对炭- co2气化行为、反应动力学和碳结构的研究,揭示了影响反应动力学的内在因素。炭的碳转化率和最大转化率受原料种类、制炭温度、灰分比例、灰分中钾含量和炭的碳结构等因素的影响。CS炭- co2反应主要受碱组分的催化作用,而PS炭的气化反应主要受孔结构的影响。等转化动力学分析表明,在碳转化率为0.5时,气化反应趋于稳定。随后,计算了初始气化温度至转化率达到50%温度的分段动力学参数。结果表明,较高的初始气化温度增加了炭- co2气化障碍,使反应难以启动,但加快了反应速率。碳的结构分析进一步阐明了反应活化能与碳的微晶结构高度相关,而反应速率更多地取决于碳的孔隙结构。
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引用次数: 4
Interface engineering of Fe-Co3N/CoP composite with N-doped C by using soybean: Fabrication of efficient electrocatalysts for oxygen evolution reaction 大豆n掺杂C Fe-Co3N/CoP复合材料的界面工程:高效析氧电催化剂的制备
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2022.12.005
Longqing Gao , Xiumin Li , Chao Tang , Tianshuo Xie , Zhengkun Xie , Haimei Li , Guoqing Guan , Jie Liu , Keyong Tang

Soybean can serve as an efficient carbon and nitrogen source for in-situ fabrication of efficient composite electrocatalysts with conductive nitrogen-doped carbon (N-C) material. In this study, the iron-doped cobalt nitride/phosphide (Fe-Co3N/CoP) nanosheet was composited with a conductive N-C material by using soybean as C and N source, as well as NH3 as additional nitrogen source. During the nitridation process of Fe-Co3N, N-C bond was formed as a newly generated Co(Fe)-N-C active sites. Therefore, it fabricates a good microscopic contact interface between the catalyst and carbon material for charge transfer. Besides, the introduction of Fe-CoP by partially phosphating Fe-Co3N further improved the OER activity due to the high catalytic activity of Co sites with high valence state. As a result, the obtained electrocatalyst exhibited overpotentials as low as 285 and 390 mV for supporting 10 and 100 mA/cm−2 current densities. This work indicates that the design of materials with good interfaces could be an effective approach for the preparation of electrocatalysts for water electrolysis.

大豆可以作为一种有效的碳和氮源,用于原位制备具有导电氮掺杂碳(N-C)材料的高效复合电催化剂。在本研究中,以大豆为碳和氮源,以及NH3为额外的氮源,将铁掺杂的氮化钴/磷化物(Fe-Co3N/CoP)纳米片与导电的N-C材料复合。在Fe-Co3N的氮化过程中,形成了新生成的Co(Fe)-N-C活性位的N-C键。因此,它在催化剂和碳材料之间制造了良好的微观接触界面,用于电荷转移。此外,通过部分磷化Fe-Co3N引入Fe-CoP,由于高价态Co位点的高催化活性,进一步提高了OER活性。因此,所获得的电催化剂在支持10和100 mA/cm−2电流密度时表现出低至285和390 mV的过电势。这项工作表明,设计具有良好界面的材料可能是制备水电解电催化剂的有效途径。
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引用次数: 0
Carposome productivity of Pleurotus ostreatus and Pleurotus eryngii growing on agro-industrial residues enriched with nitrogen, calcium salts and oils 在富含氮、钙盐和油的农工残余物上生长的平菇和羊角平菇的糖体产量
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2023.02.001
Marianna Dedousi , Eirini-Maria Melanouri , Panagiota Diamantopoulou

The suitability of the abundant agro-industrial residues wheat straw (WS; control), barley and oats straw (BOS) and rice husk (RH), supplemented with various sources of oils (sunflower, corn oil), nitrogen (peptone, yeast extract) and calcium salts (CaSO4·2H2O, CaCl2), as novel substrates in solid-state fermentation of selected Pleurotus ostreatus and P. eryngii mushrooms was investigated. The possible effect of different additives on mycelial growth rate, biomass production and endoglucanase, laccase and lipase biosynthesis were evaluated. Moreover, their impact on essential cultivation aspects (earliness, total mushroom yield, biological efficiency) and carposome quality parameters (weight, morphological characteristics) was assessed. Both fungi showed their highest growth rates on BOS substrates and the most positive implementation was CaSO4·2H2O 6 % w/w (Kr = 9.58 mm/ day; P. ostreatus, Kr = 9.42 mm/ day; P. eryngii), while different additives led to enhancement of biomass production. Pleurotus species demonstrated minimal levels of endoglucanase activity, with values ranging from 0.01 to 0.42 U/g of dry weight, regardless of the substrate and the stage of colonization. On the contrary, the maximum values of laccase activity were observed at 50 % of colonization on BOS and RH, while supplementation with nitrogen and calcium sources positively affected its biosynthesis. P. ostreatus and P. eryngii cultivated on BOS supplemented with peptone at 2 and 5 % w/w, synthesized significant laccase amounts, i.e., 12,165.78 and 8,624.55 U/g d.w., respectively. Satisfactory amounts of lipase were produced, especially in substrates supplemented with sunflower 2 % w/w, in quantities up to 1.42 U/g d.w., whereas the highest lipase activity was achieved by P. eryngii on WS supplemented with corn oil at 2 % w/w, with a value of 4.25 U/g d.w. being recorded. Regarding fermentation of Pleurotus species in polypropylene bags, WS and BOS supported faster colonization and shorter earliness period than RH substrates, whereas supplementation did not seem to affect these culture parameters. Furthermore, oils supplementation had a positive effect on BE of both species, with values up to 100 % for P. ostreatus and 80 % for P. eryngii on WS and BOS, whereas on RH the lowest BE values were detected. Morphological characteristics were not significantly affected by the additives. Results indicate the positive impact that certain additives have on mushroom productivity and production of enzymes with great financial and environmental importance.

丰产农工秸秆的适宜性研究研究了在对照、大麦和燕麦秸秆(BOS)和稻壳(RH)的基础上,添加不同来源的油脂(向日葵油、玉米油)、氮(蛋白胨、酵母提取物)和钙盐(CaSO4·2H2O、CaCl2)作为新型底物,对选定的平菇(Pleurotus ostreatus)和P. eryngii蘑菇进行固态发酵。考察了不同添加剂对菌丝生长速率、生物量及内切葡聚糖酶、漆酶和脂肪酶生物合成的影响。此外,还评估了它们对栽培基本方面(早熟性、蘑菇总产量、生物效率)和碳质体质量参数(重量、形态特征)的影响。两种真菌在BOS基质上均表现出最高的生长速率,其中CaSO4·2H2O 6% w/w (Kr = 9.58 mm/ day;平头扁豆,Kr = 9.42 mm/ day;而不同的添加剂对生物量产量有促进作用。侧耳菌的内切葡聚糖酶活性最低,无论底物和定殖阶段如何,其值在0.01 ~ 0.42 U/g干重之间。相反,在BOS和RH上定殖50%时,漆酶活性达到最大值,而添加氮和钙源对其生物合成有积极影响。在添加蛋白胨为2%和5% w/w的BOS培养基上培养的平叶假单胞菌(P. ostreatus)和双歧假单胞菌(P. eyngii)合成的漆酶量显著,分别为12165.78和8624.55 U/g d.w。在添加2% w/w向日葵的培养基中,脂肪酶的产量达到了令人满意的1.42 U/g d.w.,而在添加2% w/w玉米油的培养基中,双歧杆菌的脂肪酶活性最高,达到了4.25 U/g d.w.。在聚丙烯袋中发酵平菇时,WS和BOS比RH基质的定殖速度更快,早期期更短,而添加物似乎对这些培养参数没有影响。此外,添加油脂对两种物种的BE都有积极影响,在WS和BOS上,P. ostreatus的BE值高达100%,P. eyngii的BE值高达80%,而在RH上则检测到最低的BE值。形态学特征不受添加剂的显著影响。结果表明,某些添加剂对蘑菇产量和酶的生产具有积极的影响,具有重要的经济和环境意义。
{"title":"Carposome productivity of Pleurotus ostreatus and Pleurotus eryngii growing on agro-industrial residues enriched with nitrogen, calcium salts and oils","authors":"Marianna Dedousi ,&nbsp;Eirini-Maria Melanouri ,&nbsp;Panagiota Diamantopoulou","doi":"10.1016/j.crcon.2023.02.001","DOIUrl":"10.1016/j.crcon.2023.02.001","url":null,"abstract":"<div><p>The suitability of the abundant agro-industrial residues wheat straw (WS; control), barley and oats straw (BOS) and rice husk (RH), supplemented with various sources of oils (sunflower, corn oil), nitrogen (peptone, yeast extract) and calcium salts (CaSO<sub>4</sub>·2H<sub>2</sub>O, CaCl<sub>2</sub>), as novel substrates in solid-state fermentation of selected <em>Pleurotus ostreatus</em> and <em>P. eryngii</em> mushrooms was investigated. The possible effect of different additives on mycelial growth rate, biomass production and endoglucanase, laccase and lipase biosynthesis were evaluated. Moreover, their impact on essential cultivation aspects (earliness, total mushroom yield, biological efficiency) and carposome quality parameters (weight, morphological characteristics) was assessed. Both fungi showed their highest growth rates on BOS substrates and the most positive implementation was CaSO<sub>4</sub>·2H<sub>2</sub>O 6 % w/w (Kr = 9.58 mm/ day; <em>P. ostreatus</em>, Kr = 9.42 mm/ day; <em>P. eryngii</em>), while different additives led to enhancement of biomass production. <em>Pleurotus</em> species demonstrated minimal levels of endoglucanase activity, with values ranging from 0.01 to 0.42 U/g of dry weight, regardless of the substrate and the stage of colonization. On the contrary, the maximum values of laccase activity were observed at 50 % of colonization on BOS and RH, while supplementation with nitrogen and calcium sources positively affected its biosynthesis. <em>P. ostreatus</em> and <em>P. eryngii</em> cultivated on BOS supplemented with peptone at 2 and 5 % w/w, synthesized significant laccase amounts, i.e., 12,165.78 and 8,624.55 U/g d.w., respectively. Satisfactory amounts of lipase were produced, especially in substrates supplemented with sunflower 2 % w/w, in quantities up to 1.42 U/g d.w., whereas the highest lipase activity was achieved by <em>P. eryngii</em> on WS supplemented with corn oil at 2 % w/w, with a value of 4.25 U/g d.w. being recorded. Regarding fermentation of <em>Pleurotus</em> species in polypropylene bags, WS and BOS supported faster colonization and shorter earliness period than RH substrates, whereas supplementation did not seem to affect these culture parameters. Furthermore, oils supplementation had a positive effect on BE of both species, with values up to 100 % for <em>P. ostreatus</em> and 80 % for <em>P. eryngii</em> on WS and BOS, whereas on RH the lowest BE values were detected. Morphological characteristics were not significantly affected by the additives. Results indicate the positive impact that certain additives have on mushroom productivity and production of enzymes with great financial and environmental importance.</p></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"6 2","pages":"Pages 150-165"},"PeriodicalIF":6.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43942706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 7
Waste pulp chemical-looping gasification using Ni-modified electroplating sludge as an oxygen carrier 镍改性电镀污泥作氧载体的废纸浆化学循环气化
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-06-01 DOI: 10.1016/j.crcon.2022.12.002
Genyang Tang , Jing Gu , Guoqiang Wei , Haoran Yuan , Yong Chen

Waste pulp (WP) is a typical byproduct of paper industry, and Chemical-looping gasification (CLG) as a recently developed technology is highly suited to dispose high-volatile wastes like WP. In order to make a high-efficiency oxygen carrier (OC) for CLG of WP, the Ni-containing electroplating sludge (NES) was used as the matrix and NiO modification was performed to enhance the hydrogen production in CLG. These resulted in a potentially high-efficiency OC denoted as NNES. Testing CLG of WP was in a fixed-bed reactor at 850 °C by adopting NNES as the OC, injecting 2.4 mL/g(WP) water, and keeping a mass ratio of 1.0 between OC to WP. It produced 1.73 Nm3/kg syngas that has an LHV of 11.9 MJ/Nm3 and a H2/CO ratio of 3.63. In 10 redox cycles, the syngas yield did not have obvious decrease, but a certain reduction in the activity of NNES was observed. Characterization of the spent NNES revealed that it is the Ni agglomeration and inert silicate generation which reduced the activity of NNES.

废纸浆是造纸工业的典型副产物,而化学循环气化技术是近年来发展起来的一项非常适合处理废纸浆等高挥发性废弃物的技术。为制备高效氧载体(OC),以含镍电镀污泥(NES)为基体,对其进行NiO改性,提高CLG的产氢率。这就产生了一种潜在的高效率OC,称为NNES。在850℃的固定床反应器中,以NNES为OC,注入2.4 mL/g(WP)的水,OC与WP的质量比为1.0,测试WP的CLG。产气量为1.73 Nm3/kg, LHV为11.9 MJ/Nm3, H2/CO比为3.63。在10个氧化还原循环中,合成气产量没有明显下降,但NNES活性有一定的降低。废NNES的表征表明,Ni的团聚和惰性硅酸盐的生成降低了NNES的活性。
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引用次数: 1
Selectivity of CO2 reduction reaction to CO on the graphitic edge active sites of Fe-single-atom and dual-atom catalysts: A combined DFT and microkinetic modeling Fe单原子和双原子催化剂石墨边缘活性位点上CO2还原CO反应的选择性:DFT和微观动力学模型
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-05-18 DOI: 10.1016/j.crcon.2023.05.004
Ahmad Nuruddin , Adhitya Gandaryus Saputro , Arifin Luthfi Maulana , Febdian Rusydi , Fiki Taufik Akbar , Hadi Teguh Yudistira , Hermawan Kresno Dipojono

We study the carbon dioxide reduction reaction (CO2RR) activity and selectivity of Fe single-atom catalyst (Fe-SAC) and Fe dual-atom catalyst (Fe-DAC) active sites at the interior of graphene and the edges of graphitic nanopore by using a combination of DFT calculations and microkinetic simulations. The trend of limiting potentials for CO2RR to produce CO can be described by using either the adsorption energy of COOH, CO, or their combination. CO2RR process with reasonable reaction rates can be achieved only on the active site configurations with weak tendencies toward CO poisoning. The efficiency of CO2RR on a catalyst depends on its ability to suppress the parasitic hydrogen evolution reaction (HER), which is directly related to the behavior of H adsorption on the catalyst’s active site. We find that the edges of the graphitic nanopore can act as potential adsorption sites for an H atom, and in some cases, the edge site can bind the H atom much stronger than the main Fe site. The linear scaling between CO and H adsorptions is broken if this condition is met. This condition also allows some edge active site configurations to have their CO2RR limiting potential lower than the HER process favoring CO production over H2 production.

采用DFT计算和微动力学模拟相结合的方法,研究了石墨烯内部和石墨纳米孔边缘的铁单原子催化剂(Fe- sac)和铁双原子催化剂(Fe- dac)活性位点的二氧化碳还原反应(CO2RR)活性和选择性。CO2RR生成CO的极限电位趋势可以用COOH、CO或它们组合的吸附能来描述。只有在CO中毒倾向较弱的活性位点构型上才能实现合理反应速率的CO2RR过程。CO2RR在催化剂上的效率取决于其抑制寄生析氢反应(HER)的能力,而寄生析氢反应的抑制能力与催化剂活性位点对H的吸附行为直接相关。我们发现石墨纳米孔的边缘可以作为H原子的潜在吸附位点,并且在某些情况下,边缘位点对H原子的结合能力比主要的Fe位点强得多。如果满足这个条件,CO和H吸附之间的线性标度被打破。这种情况还允许一些边缘活性位点配置的CO2RR极限电位低于HER工艺,有利于CO的产生而不是H2的产生。
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引用次数: 0
Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions 含混相前驱体钯改性CuO-ZnO-Al2O3催化剂温和条件下CO2加氢合成甲醇
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-05-16 DOI: 10.1016/j.crcon.2023.05.003
Xiao Fan , Kaiying Wang , Xiaoqing He , Shiguang Li , Miao Yu , Xinhua Liang

A series of palladium-modified (Pd-modified) CuO-ZnO-Al2O3 (CZA) catalysts with various Pd loadings (0.3 wt% to 2.4 wt%) were prepared using the wetness impregnation method, on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases (CZA-zH), and CuO-ZnO-Al2O3 metal oxide nanoparticles (CZA-MO). Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180–240 °C for methanol synthesis via CO2 hydrogenation. Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180 °C for 100 hrs of reaction. The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups (e.g., –OH) of CZA-zH support, which is beneficial for better adsorption and distribution of Pd promoter. Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO, and peak shift of Cu to a lower binding energy. The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction conditions.

采用湿浸渍法制备了钯改性(Pd改性)CuO-ZnO-Al2O3 (CZA)催化剂,催化剂的Pd负载量在0.3 wt% ~ 2.4 wt%之间。CZA载体为两种不同结构的CZA载体,分别是由锌-孔雀石和类水滑石相混合组成的CZA- zh前驱体和CuO-ZnO-Al2O3金属氧化物纳米颗粒(CZA- mo)。在180 ~ 240℃的温度范围内,pd修饰的CZA催化剂对CO2加氢合成甲醇的催化活性均有增强。Pd/CZA-zH催化剂在180℃的较低反应温度下,反应时间为100小时,制备甲醇的效率更高、更稳定。活性的提高主要是由于CZA-zH载体具有更高的表面积和丰富的含氧官能团(如-OH),有利于Pd促进剂更好的吸附和分布。氢温度程序还原和x射线光电子能谱结果表明,Pd和Cu在Pd/CZA-zH催化剂上通过增强CuO的还原性和Cu的峰移到更低的结合能而更好地相互作用。钯促进剂在两种CZA载体上的氢溢出效应利用率不同,导致两种CZA载体在温和反应条件下的甲醇合成性能不同。
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引用次数: 1
Co-production of hydrochar and bioactive compounds from Ulva lactuca via a hydrothermal process 水热法从羊茅中联合生产水炭和生物活性化合物
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-05-16 DOI: 10.1016/j.crcon.2023.05.002
Edy Hartulistiyoso , Obie Farobie , Latifa A Anis , Novi Syaftika , Asep Bayu , Apip Amrullah , Navid R. Moheimani , Surachai Karnjanakom , Yukihiko Matsumura

This study investigates the simultaneous production of hydrochar and bioactive compounds from Ulva lactuca via a hydrothermal process. The experiment was carried out using a batch reaction vessel at different reaction temperatures of 180–220 °C and various holding times of 30–90 min. As expected, both temperature and time vigorously influenced hydrochar and bioactive compound production. The maximum hydrochar yield was at 32.4 wt%. The higher heating value (HHV) of hydrochar was observed in the range of 17.68–21.07 MJ kg−1, near the energy content of low-rank coals. The hydrochars exhibited contact angles higher than 90° (i.e., 94-108°) for a longer time, confirming their hydrophobic surfaces. The scanning electron microscope analysis (SEM) showed that the hydrothermal process enables cracks in the spherical shape of raw U. lactuca into small and porous particles. Besides producing hydrochar, the hydrothermal process of U. lactuca also gives promising antioxidants and phenolics as bioactive compounds. The highest total phenolic content and antioxidant activity could be achieved in hydrolysate at 200 °C and 30 min with the value of 1.20 ± 0.12 mg/g and 71.6 ± 1.3%, respectively.

本研究探讨了水热法同时生产乳酸Ulva的碳氢化合物和生物活性化合物。实验采用间歇式反应容器,在180-220℃的不同反应温度和30-90 min的不同保温时间下进行。正如预期的那样,温度和时间对碳氢化合物和生物活性化合物的生产都有很大影响。最大烃类产率为32.4%。煤的热值(HHV)在17.68 ~ 21.07 MJ kg−1之间,接近低阶煤的能量含量。接触角大于90°(即94 ~ 108°)的时间较长,证实了其疏水表面。扫描电镜(SEM)分析表明,热液作用使原乳酸菌的球形裂纹变为小而多孔的颗粒。除了产生碳氢化合物外,乳藻土的水热过程还可以产生具有生物活性的抗氧化剂和酚类化合物。水解产物在200℃、30 min时总酚含量和抗氧化活性最高,分别为1.20±0.12 mg/g和71.6±1.3%。
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