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Nitrogen-functionalized modulation of iron nanoparticles promotes selective hydrogenation of carbon dioxide 铁纳米颗粒的氮功能化调制促进了二氧化碳的选择性氢化
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.09.010
Xianbiao Wang , Jun Qian , Zixuan Lu , Jie Huang , Liru Zheng , Yong Jiang , Mengdie Cai , Yuxue Wei , Lisheng Guo , Song Sun
Nitrogen-functionalized iron nanoparticles were prepared using a one-pot hydrothermal process. The utilization of urea as a nitrogen source during the hydrothermal process significantly influenced the morphology and defects of the obtained catalyst. Within an optimal range, the actual nitrogen promoter content could be controlled by altering the amount of urea introduced. The presence of a nitrogen promoter not only impacts catalytic activity but also plays a crucial role in product distribution. The FeC-N catalyst exhibited 32.0% selectivity toward light olefins, with a CO2 conversion of 26.8%. The improvement in catalytic performance correlated with the specific surface area, dispersion of iron species, number of defect sites, and content of pyrrolic N species. Moreover, the enhanced selectivity for light olefins can be attributed to easier desorption from the FeC-N catalyst, thereby avoiding the over-hydrogenation of light olefins to paraffins.
采用一锅水热法制备了氮官能化铁纳米颗粒。水热过程中尿素作为氮源的利用对催化剂的形貌和缺陷有显著影响。在最佳范围内,可以通过改变尿素的添加量来控制氮促进剂的实际含量。氮启动子的存在不仅影响催化活性,而且在产物分布中起着至关重要的作用。FeC-N催化剂对轻烯烃的选择性为32.0%,CO2转化率为26.8%。催化性能的提高与比表面积、铁的分散性、缺陷位的数量和吡咯态氮的含量有关。此外,轻质烯烃选择性的增强可归因于更容易从FeC-N催化剂上解吸,从而避免了轻质烯烃过度加氢生成石蜡。
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引用次数: 0
Enhancing perovskite/silicon tandem solar cells via nuclei engineering 通过核工程增强钙钛矿/硅串联太阳能电池
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.09.006
Dongyang Li , Xinyu Jiang , Peter Müller-Buschbaum , Ruijie Ma , Gang Li
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引用次数: 0
Rational design of H2 production sites for achieving photoconversion of CO2 with H2O into widely adjustable syngas and highly effective H2 evolution 合理设计产氢位点,实现CO2与H2O光转化为可广泛调节的合成气和高效的氢气析出
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.07.008
Guoqiang Zhang , Zhiqi Wang , Diandian Shi , Guangbo Liu , Tao He , Jingli Wu , Jinzhi Zhang , Jinhu Wu
The photoconversion of CO2 with H2O into widely tunable syngas (CO and H2) or pure H2 production is regarded as a promising strategy to mitigate escalating energy shortages and climate change. Herein, anchoring the H2 production sites onto the surface of CdIn2S4 (CIS) with a nanoscale hollow sphere allows for the photoconversion of CO2 into syngas and water splitting to H2. The CO/H2 ratio can be realized in a remarkably wide range from 1:0.38 to 1:3.76. The optimized CIS/Co-PBA/NaY-5 hybrid exhibits superior photocatalytic syngas evolution up to 1458.48 μmol·g−1·h−1 (H2/CO, 1152.29/306.19 μmol·g−1·h−1), and the H2 evolution rate increases by 431.70% compared with CIS. The CIS/Co-PBA/NaY-5 hybrid exhibited not only superior H2 evolution but also recyclability. The experimental, energy-dispersive X-ray spectroscopy, and electron spin resonance results indicate that the Co sites serve as H2 production sites and promote the H2 evolution reaction. In addition, the construction of a p-n heterojunction with a special micromorphology is beneficial for the separation/transfer of carriers.
二氧化碳与水的光转化为广泛可调的合成气(CO和H2)或纯H2生产被认为是缓解日益严重的能源短缺和气候变化的一种有前途的策略。在这里,用纳米级中空球体将H2生成位点锚定在CdIn2S4 (CIS)表面上,允许CO2光转化为合成气,水分解为H2。CO/H2比可以在1:0.38到1:3.76的非常宽的范围内实现。优化后的CIS/ CO - pba /NaY-5复合物的光催化合成气析出率为1458.48 μmol·g−1·h−1 (H2/CO为1152.29/306.19 μmol·g−1·h−1),H2的析出率比CIS提高了431.70%。CIS/Co-PBA/NaY-5杂合物不仅具有较好的析氢性能,而且具有可回收性。实验、能量色散x射线光谱和电子自旋共振结果表明,Co位点作为H2生成位点,促进H2的析出反应。此外,具有特殊微形貌的p-n异质结的构建有利于载流子的分离/转移。
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引用次数: 0
Recent advances in microalgae-driven carbon capture, utilization, and storage: Strain engineering through adaptive laboratory evolution and microbiome optimization 微藻驱动的碳捕获、利用和储存的最新进展:通过适应性实验室进化和微生物组优化的菌株工程
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.10.001
Zhongshi He , Jing Wang , Yantao Li
The potential of microalgae as a biological resource for carbon capture, utilization, and storage (CCUS) has been extensively discussed. Although genetic engineering methods have been employed to improve microalgal phenotypes, they often face challenges related to public concerns regarding genetically modified organisms. By contrast, adaptive laboratory evolution (ALE) and microbiome optimization have emerged as promising non-genetic modification strategies, with notable success in bacterial models. In microalgae, ALE has been employed to improve resilience against varying environmental and stress factors and increase carbon capture efficiency, and for the production of valuable bioproducts through gradual accumulation of beneficial mutations following manual or automated selection. Furthermore, advancements in the understanding of microbial symbiotic relationships in the phycosphere have facilitated microbiome optimization in microalgal cultivation systems, significantly improving their functionality and productivity. In this study, we provide a comprehensive overview of the latest advancements in ALE and microbiome optimization of microalgae for CCUS across different carbon emission scenarios, including flue gas, biogas, wastewater, and landfill leachate. We further discuss the current challenges and future directions for the integration of ALE with microbiome optimization, focusing on the potential synergies of these methodologies. Overall, ALE and microbiome optimization are promising approaches to direct microalgae for environmental and industrial CCUS applications, thereby reducing global carbon emissions and addressing climate change challenges.
微藻作为碳捕获、利用和封存(CCUS)生物资源的潜力已被广泛讨论。虽然基因工程方法已被用于改善微藻表型,但他们经常面临与公众对转基因生物的关注相关的挑战。相比之下,适应性实验室进化(ALE)和微生物组优化已成为有前途的非基因修饰策略,在细菌模型中取得了显著成功。在微藻中,ALE已被用于提高对各种环境和应激因素的抵御能力,提高碳捕获效率,并通过手动或自动选择的有益突变的逐渐积累来生产有价值的生物产品。此外,对藻圈中微生物共生关系的理解的进步促进了微藻培养系统中微生物组的优化,显着提高了它们的功能和生产力。在本研究中,我们全面概述了在不同碳排放情景下(包括烟气、沼气、废水和垃圾渗滤液)CCUS中微藻的ALE和微生物组优化的最新进展。我们进一步讨论了ALE与微生物组优化整合的当前挑战和未来方向,重点是这些方法的潜在协同作用。总体而言,ALE和微生物组优化是指导微藻用于环境和工业CCUS应用的有前途的方法,从而减少全球碳排放,应对气候变化挑战。
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引用次数: 0
Alcohol pretreatment for depolymerization and fractionation of corn stalk 玉米秸秆醇预处理解聚分馏研究
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.09.005
Lijuan Gao , Wentao Li , Yu Zhang , Meijing Wang , Wen Wang , Cuiyi Liang , Shiyou Xing , Wei Qi
The development of an efficient pretreatment technology to depolymerize and fractionate lignocellulose into glucan, xylan, and lignin is crucial for lignocellulose biorefinery. In this study, alcohol pretreatments using methanol and pentanol were developed and compared. Based on the solubility of the two alcohols, the methanol and pentanol pretreatments are homogeneous and biphasic, respectively. Carbon flow analysis revealed that 1 kg of corn stalk (CS) yielded 111.9 g of lignin with the homogeneous pretreatment (lignin yield: 60.0%), while 149.8 g of lignin was obtained with the biphasic pretreatment (lignin yield: 80.3%). Biphasic pretreatment yielded the lignin with higher activity (more β-O-4 bond content). Additionally, 210.4 g and 267.0 g of glucose were obtained from the enzymatic hydrolysis of homogeneously and biphasically pretreated CS, respectively, where glucose yields were 53.0% and 67.2%, respectively. Fourier Transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) were employed to verify the component fractionation results. The Hansen solubility parameter and combined severity factor analysis were used to evaluate the effects of various factors on component fractionation. Nuclear magnetic resonance and mechanistic analyses were performed to explore the process of component fractionation. Overall, we discovered that biphasic pretreatment was significantly better than homogeneous pretreatment in component fractionation, including component recovery and lignin activity.
开发一种有效的预处理技术,将木质纤维素解聚和分馏成葡聚糖、木聚糖和木质素,是木质纤维素生物精制的关键。研究了甲醇和戊醇的醇前处理方法,并进行了比较。根据两种醇的溶解度,甲醇和戊醇预处理分别为均相和双相。碳流分析结果表明,1 kg玉米秸秆均相预处理的木质素产率为111.9 g(木质素产率为60.0%),而两相预处理的木质素产率为149.8 g(木质素产率为80.3%)。双相预处理得到的木质素具有较高的活性(β-O-4键含量较高)。此外,均相预处理和双相预处理CS的酶解葡萄糖分别为210.4 g和267.0 g,葡萄糖产率分别为53.0%和67.2%。采用傅里叶变换红外光谱(FT-IR)和x射线衍射(XRD)对组分的分馏结果进行了验证。采用Hansen溶解度参数和联合严重程度因子分析评价了各因素对组分分馏的影响。通过核磁共振和机理分析对组分分馏过程进行了探讨。总的来说,我们发现双相预处理在组分分馏方面明显优于均相预处理,包括组分回收率和木质素活性。
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引用次数: 0
Direct synthesis of alkyl amines from dinitrogen and alkenes 二氮和烯烃直接合成烷基胺
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.08.002
Jinhui Wang , Yanwei Cao , Cuijuan Zhang , Lin He , Jiaxiang Chu
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引用次数: 0
Breaking the stability limit of zeolite-based alkane dehydrogenation catalysts 突破沸石基烷烃脱氢催化剂的稳定性极限
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.07.006
Zhiqiang Liu , Anmin Zheng
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引用次数: 0
Efficient atomically dispersed Fe catalysts with robust three-phase interface for stable seawater-based zinc-air batteries 具有坚固三相界面的高效原子分散铁催化剂用于稳定的海水基锌-空气电池
Pub Date : 2025-03-01 DOI: 10.1016/j.greenca.2024.09.002
Daokun Kang , Canhui Zhang , Xingkun Wang , Fanqi Wang , Huiyu Gai , Hanxu Yao , Xu Liu , Zhuangzhuang He , Minghua Huang , Heqing Jiang
The use of seawater-based electrolytes in zinc-air batteries (S-ZABs) presents significant economic and social benefits and mitigates the demand for scarce freshwater resources. However, it is challenging to achieve a metal–nitrogen–carbon (M–N–C) catalyst that exhibits high resistance to corrosive Cl in seawater-based electrolytes and possesses a strengthened binding affinity with O2, which enables catalysts with an optimized oxygen reduction reaction (ORR) and enhances the applicability of S-ZABs. Herein, we propose a combined wet chemistry-pyrolysis strategy to obtain atomically dispersed Fe-decorated nitrogen-doped mesoporous carbon spheres (N-MCS-Fe-900). Benefiting from the capacity of the Fe decorations to form the edge-hosted aerophilic FeN4-O2 sites at the optimized three-phase interface, N-MCS-Fe-900 affords the enhanced resistance of the active Fe sites to corrosive Cl, as well as improved interaction with O2, thereby facilitating the ORR process. As expected, the N-MCS-Fe-900 delivers high half wave potential of 0.90 V and kinetic current density of 18.61 mA cm−2 at 0.85 V in seawater-based 0.1 M KOH. More importantly, the S-ZABs equipped with N-MCS-Fe-900 exhibited long-term stability under a high current density for over 140 h without voltage decay. Theoretical calculations and electrochemical performance evaluations collectively revealed the superior catalytic efficacy and genesis of this activity in N-MCS-Fe-900, which features edge-hosted FeN4-O2 sites at the stable three-phase interface in seawater electrolytes. This study provides new insights for the advancement of ORR catalysts in sustainable energy conversion technologies for seawater-based electrolytes.
在锌空气电池(S-ZABs)中使用海水电解质具有显著的经济和社会效益,并减轻了对稀缺淡水资源的需求。然而,在海水基电解质中,金属-氮-碳(M-N-C)催化剂既具有较高的耐腐蚀性Cl -,又具有较强的与O2的结合亲和力,从而使催化剂具有优化的氧还原反应(ORR),增强S-ZABs的适用性,这是一个挑战。在此,我们提出了一种湿化学-热解相结合的策略来获得原子分散的fe修饰的氮掺杂介孔碳球(N-MCS-Fe-900)。N-MCS-Fe-900得益于Fe修饰物在优化的三相界面上形成边缘承载的亲氧FeN4-O2位点的能力,增强了活性Fe位点对腐蚀性Cl -的抵抗力,并改善了与O2的相互作用,从而促进了ORR过程。正如预期的那样,N-MCS-Fe-900在海水基0.1 M KOH中提供0.90 V的高半波电位和0.85 V时18.61 mA cm−2的动态电流密度。更重要的是,配备N-MCS-Fe-900的S-ZABs在高电流密度下表现出超过140 h的长期稳定性,没有电压衰减。理论计算和电化学性能评估共同揭示了N-MCS-Fe-900在海水电解质稳定三相界面上具有边缘负载的FeN4-O2位点的优越催化效果和该活性的原因。该研究为ORR催化剂在海水基电解质可持续能量转换技术中的应用提供了新的思路。
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引用次数: 0
One-pot conversion of cellulosic sugars into methyl lactate using hierarchical Sn-MFI zeolite with intracrystalline mesoporosity 利用具有晶内介孔的分级Sn-MFI沸石一锅法将纤维素糖转化为乳酸甲酯
Pub Date : 2024-12-01 DOI: 10.1016/j.greenca.2024.06.007
Yuying Li , Xiumei Liu , Kun Zhang , Siyuan Zhao , Lei Wu , Qiang Guo , Hong Du , Feng Wang
Cellulosic sugars derived from lignocellulose are the most abundant and inexpensive raw materials used for the production of methyl lactate (MLA). In this study, hierarchical Sn-MFI zeolite with intracrystalline mesoporosity was developed, capable of catalyzing the one-pot conversion of cellulosic sugars into MLA in a CH3OH/H2O mixture. The MLA yield from glucose using the hierarchical Sn-MFI zeolite was almost twice as high as that using the conventional microporous Sn-MFI zeolite. This superior catalytic performance was attributed to the reduced diffusion limitation of glucose within the hierarchical Sn-MFI catalyst, which possessed significant intercrystalline mesoporosity. Additionally, the hierarchical Sn-MFI catalyst was recycled for five reaction runs of the one-pot conversion of glucose without an obvious loss of activity, indicating excellent stability and reusability and broadening the scope of carbohydrates used to obtain MLA.
从木质纤维素中提取的纤维素糖是用于生产乳酸甲酯(MLA)的最丰富和最便宜的原料。在本研究中,开发了具有晶内介孔的分级Sn-MFI沸石,能够在CH3OH/H2O混合物中催化纤维素糖一锅转化为MLA。使用分级Sn-MFI沸石从葡萄糖中提取MLA的收率几乎是使用常规微孔Sn-MFI沸石的两倍。这种优异的催化性能归因于葡萄糖在分级Sn-MFI催化剂中的扩散限制降低,该催化剂具有显着的晶间介孔。此外,层次化Sn-MFI催化剂在一锅转化葡萄糖的五次反应中没有明显的活性损失,表明了良好的稳定性和可重复使用性,扩大了用于获得MLA的碳水化合物的范围。
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引用次数: 0
Enhancing the performance of spinel La-doped CoFe2O4 oxygen carriers for chemical looping hydrogen generation 提高尖晶石la掺杂CoFe2O4氧载体化学环制氢性能
Pub Date : 2024-12-01 DOI: 10.1016/j.greenca.2024.08.004
Weifeng Song , Jingli Wu , Jianqing Li , Zhiqi Wang , Tao He , Wenqing Chen , Deshuai Sun , Jinhu Wu
Chemical-looping hydrogen generation (CLHG) is a clean and efficient method for sustainable hydrogen production. The industrial advancement of the CLHG technology hinges on the development of highly active and selective oxygen carriers (OCs). In this study, the performances of three spinel OCs (ZnFe2O4, CoFe2O4, and NiFe2O4) were investigated in a fixed-bed reactor. CoFe2O4 demonstrated the best reactivity and highest hydrogen yield. In addition, doping CoFe2O4 with varying amounts of La further improved its performance. The highest hydrogen yield (393 mL/g) was observed for CoFe2O4 doped with 10% by mass of La. The characterization results indicated that La not only facilitated the formation of oxygen vacancies but also accelerated lattice oxygen transfer. Furthermore, an optimized La doping level was found to boost the crystallinity of the oxygen carrier, leading to improved cycling performance. The insights gained from probing the performance of La-doped CoFe2O4 OCs are expected to contribute to the development of novel OCs for scaled-up CLHG technology.
化学环制氢(CLHG)是一种清洁高效的可持续制氢方法。高活性、高选择性氧载体(OCs)的发展是CLHG技术产业化发展的关键。在固定床反应器中,研究了三种尖晶石OCs (ZnFe2O4、CoFe2O4和NiFe2O4)的性能。CoFe2O4表现出最好的反应活性和最高的产氢率。此外,掺杂不同量的La的CoFe2O4进一步提高了其性能。当La质量分数为10%时,CoFe2O4的产氢率最高,为393 mL/g。表征结果表明,La不仅促进了氧空位的形成,而且加速了晶格氧的转移。此外,优化的La掺杂水平可以提高氧载体的结晶度,从而提高循环性能。从探索la掺杂CoFe2O4 OCs的性能中获得的见解有望有助于开发用于大规模CLHG技术的新型OCs。
{"title":"Enhancing the performance of spinel La-doped CoFe2O4 oxygen carriers for chemical looping hydrogen generation","authors":"Weifeng Song ,&nbsp;Jingli Wu ,&nbsp;Jianqing Li ,&nbsp;Zhiqi Wang ,&nbsp;Tao He ,&nbsp;Wenqing Chen ,&nbsp;Deshuai Sun ,&nbsp;Jinhu Wu","doi":"10.1016/j.greenca.2024.08.004","DOIUrl":"10.1016/j.greenca.2024.08.004","url":null,"abstract":"<div><div>Chemical-looping hydrogen generation (CLHG) is a clean and efficient method for sustainable hydrogen production. The industrial advancement of the CLHG technology hinges on the development of highly active and selective oxygen carriers (OCs). In this study, the performances of three spinel OCs (ZnFe<sub>2</sub>O<sub>4</sub>, CoFe<sub>2</sub>O<sub>4</sub>, and NiFe<sub>2</sub>O<sub>4</sub>) were investigated in a fixed-bed reactor. CoFe<sub>2</sub>O<sub>4</sub> demonstrated the best reactivity and highest hydrogen yield. In addition, doping CoFe<sub>2</sub>O<sub>4</sub> with varying amounts of La further improved its performance. The highest hydrogen yield (393 mL/g) was observed for CoFe<sub>2</sub>O<sub>4</sub> doped with 10% by mass of La. The characterization results indicated that La not only facilitated the formation of oxygen vacancies but also accelerated lattice oxygen transfer. Furthermore, an optimized La doping level was found to boost the crystallinity of the oxygen carrier, leading to improved cycling performance. The insights gained from probing the performance of La-doped CoFe<sub>2</sub>O<sub>4</sub> OCs are expected to contribute to the development of novel OCs for scaled-up CLHG technology.</div></div>","PeriodicalId":100595,"journal":{"name":"Green Carbon","volume":"2 4","pages":"Pages 393-400"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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