Pub Date : 2024-08-16DOI: 10.1016/j.ccst.2024.100272
Quantum dots exhibit great potential in photocatalytic CO2 conversion into value-added fuels to achieve a carbon-neutral society, owing to their unique optical properties and tunable surface chemistry. However, the generation of multi-carbon hydrocarbon products remains a grand challenge. Herein, polyethyleneimine (PEI) coated AgInS2 quantum dots (AgInS2@PEI QDs) are designed for the photo-catalytic conversion of CO2 to C2 products. It is found that the yield and selectivity of C2H6 can be significantly enhanced by regulating the content of Ag and PEI in AgInS2@PEI QDs. Under the optimal conditions, C2H6 yield reaches 63 μmol g-1, and the electron selectivity is 30.3 %. A mechanistic study reveals that PEI effectively promotes the accumulation of photogenerated electrons, and the CO-enriched local environment caused by Ag boosts CC coupling on asymmetric bimetallic sites. This work offers new insight on the design of efficient quantum dot photocatalysts for CO2 conversion to C2 products.
量子点因其独特的光学特性和可调表面化学性质,在光催化二氧化碳转化为高附加值燃料以实现碳中和社会方面展现出巨大潜力。然而,生成多碳碳氢化合物产品仍然是一个巨大的挑战。本文设计了聚乙烯亚胺(PEI)包覆的 AgInS2 量子点(AgInS2@PEI QDs),用于光催化将 CO2 转化为 C2 产物。研究发现,通过调节 AgInS2@PEI QDs 中 Ag 和 PEI 的含量,可以显著提高 C2H6 的产率和选择性。在最佳条件下,C2H6 产率达到 63 μmol g-1,电子选择性为 30.3%。机理研究表明,PEI 能有效地促进光生电子的积累,而 Ag 带来的富含 CO 的局部环境则促进了不对称双金属位点上的 CC 耦合。这项研究为设计将 CO2 转化为 C2 产物的高效量子点光催化剂提供了新的思路。
{"title":"Polyethyleneimine coated AgInS2 quantum dots for efficient CO2 photoreduction to C2H6","authors":"","doi":"10.1016/j.ccst.2024.100272","DOIUrl":"10.1016/j.ccst.2024.100272","url":null,"abstract":"<div><p>Quantum dots exhibit great potential in photocatalytic CO<sub>2</sub> conversion into value-added fuels to achieve a carbon-neutral society, owing to their unique optical properties and tunable surface chemistry. However, the generation of multi-carbon hydrocarbon products remains a grand challenge. Herein, polyethyleneimine (PEI) coated AgInS<sub>2</sub> quantum dots (AgInS<sub>2</sub>@PEI QDs) are designed for the photo-catalytic conversion of CO<sub>2</sub> to C<sub>2</sub> products. It is found that the yield and selectivity of C<sub>2</sub>H<sub>6</sub> can be significantly enhanced by regulating the content of Ag and PEI in AgInS<sub>2</sub>@PEI QDs. Under the optimal conditions, C<sub>2</sub>H<sub>6</sub> yield reaches 63 μmol g<sup>-1</sup>, and the electron selectivity is 30.3 %. A mechanistic study reveals that PEI effectively promotes the accumulation of photogenerated electrons, and the CO-enriched local environment caused by Ag boosts C<img>C coupling on asymmetric bimetallic sites. This work offers new insight on the design of efficient quantum dot photocatalysts for CO<sub>2</sub> conversion to C<sub>2</sub> products.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000848/pdfft?md5=573f56abdb40eb17fc84f564b6c9d7a6&pid=1-s2.0-S2772656824000848-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141993146","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}
Pub Date : 2024-08-16DOI: 10.1016/j.ccst.2024.100270
Sodium carbonate solvent absorbent has been widely studied for CO2 reduction to deal with global warming because of its green, low cost, and non-corrosive advantages. However, in the application of sodium carbonate as an absorbent for CO2 capture, there is no unified cognition of the mass transfer process, which leads to the lack of guidance for the industrial large-scale process. Moreover, the mechanism of mass transfer enhancement of surfactants, which can effectively improve the mass transfer performance, has not been effectively explored in the literature. Based on this, this paper firstly adopts the molecular dynamics method to analyze the solution characteristics after surfactant addition and optimize the surfactant. Subsequently, a classical dissolved oxygen test method was used to measure the gas-liquid mass transfer coefficient for CO2 absorption into sodium carbonate solution. And based on this mass transfer coefficient measurement method, the mass transfer process of sodium carbonate solution with surfactant was analyzed. The results showed that the sodium carbonate solution with 5 wt% concentration and 10 wt% concentration at 30 °C did not satisfy the pseudo first-order fast chemical reaction kinetics assumption. To improve CO2 absorption mass transfer rate, dodecyl trimethyl ammonium chloride (DTAC) surfactant was introduced, which was improved by 119 % compared with non-enhanced solvent at 5 wt% concentration solution, and the assumption of pseudo first order fast chemical reaction was satisfied. After the introduction of surfactant, the barrier effect decreased the liquid phase mass transfer coefficient, but the Marangoni effect happened in the 5 wt% concentration of sodium carbonate solution, which enhanced the liquid-phase mass-transfer coefficient. This finding reveals the mechanism of mass transfer promotion of sodium carbonate by the surfactant DTAC, which is of great engineering significance for the application in the field of decarbonization after the introduction of surfactant.
{"title":"Carbon dioxide capture in sodium carbonate solution: Mass transfer kinetics and DTAC surfactant enhancement mechanism","authors":"","doi":"10.1016/j.ccst.2024.100270","DOIUrl":"10.1016/j.ccst.2024.100270","url":null,"abstract":"<div><p>Sodium carbonate solvent absorbent has been widely studied for CO<sub>2</sub> reduction to deal with global warming because of its green, low cost, and non-corrosive advantages. However, in the application of sodium carbonate as an absorbent for CO<sub>2</sub> capture, there is no unified cognition of the mass transfer process, which leads to the lack of guidance for the industrial large-scale process. Moreover, the mechanism of mass transfer enhancement of surfactants, which can effectively improve the mass transfer performance, has not been effectively explored in the literature. Based on this, this paper firstly adopts the molecular dynamics method to analyze the solution characteristics after surfactant addition and optimize the surfactant. Subsequently, a classical dissolved oxygen test method was used to measure the gas-liquid mass transfer coefficient for CO<sub>2</sub> absorption into sodium carbonate solution. And based on this mass transfer coefficient measurement method, the mass transfer process of sodium carbonate solution with surfactant was analyzed. The results showed that the sodium carbonate solution with 5 wt% concentration and 10 wt% concentration at 30 °C did not satisfy the pseudo first-order fast chemical reaction kinetics assumption. To improve CO<sub>2</sub> absorption mass transfer rate, dodecyl trimethyl ammonium chloride (DTAC) surfactant was introduced, which was improved by 119 % compared with non-enhanced solvent at 5 wt% concentration solution, and the assumption of pseudo first order fast chemical reaction was satisfied. After the introduction of surfactant, the barrier effect decreased the liquid phase mass transfer coefficient, but the Marangoni effect happened in the 5 wt% concentration of sodium carbonate solution, which enhanced the liquid-phase mass-transfer coefficient. This finding reveals the mechanism of mass transfer promotion of sodium carbonate by the surfactant DTAC, which is of great engineering significance for the application in the field of decarbonization after the introduction of surfactant.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000824/pdfft?md5=3d7cd906eec73fe0e741827795a124e2&pid=1-s2.0-S2772656824000824-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141993147","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}
Pub Date : 2024-08-16DOI: 10.1016/j.ccst.2024.100273
Aerosol emissions from the CO2-capture process have a significant impact on both solvent depletion and environmental contamination. This work comprehensively investigated the emissions of AMP (2-amino-2-methyl-1propanol)/PZ (piperazine) from a bench-scale platform and a CO2-capture pilot plant. The concentration of nuclei in flue gas is a key factor affecting aerosol emissions, and a high nuclei concentration leads to more serious aerosol emission problems. The amine emissions after the absorber in the three different scenarios (no added nuclei, nuclei added, and pilot plant) were 273, 1051, and 1347 mg/Nm3, respectively. Increasing the lean-solvent temperature promoted aerosol emissions, and increasing the liquid/gas ratio and CO2 loading in the lean solvent suppressed aerosol emissions. In the pilot plant, the effects of four mitigation measures were evaluated, and it was found that dry bed and acid washing had better mitigation effects than did conventional water washing; amine emissions could be reduced to as low as 21 mg/Nm3 PZ and 25 mg/Nm3 AMP. This study provides a reference for the design and optimization of carbon-dioxide-capture systems, which can help to reduce the impact on the environment.
{"title":"Aerosol emissions and mitigation of aqueous AMP/PZ solvent for postcombustion CO2 capture","authors":"","doi":"10.1016/j.ccst.2024.100273","DOIUrl":"10.1016/j.ccst.2024.100273","url":null,"abstract":"<div><p>Aerosol emissions from the CO<sub>2</sub>-capture process have a significant impact on both solvent depletion and environmental contamination. This work comprehensively investigated the emissions of AMP (2-amino-2-methyl-1propanol)/PZ (piperazine) from a bench-scale platform and a CO<sub>2</sub>-capture pilot plant. The concentration of nuclei in flue gas is a key factor affecting aerosol emissions, and a high nuclei concentration leads to more serious aerosol emission problems. The amine emissions after the absorber in the three different scenarios (no added nuclei, nuclei added, and pilot plant) were 273, 1051, and 1347 mg/Nm<sup>3</sup>, respectively. Increasing the lean-solvent temperature promoted aerosol emissions, and increasing the liquid/gas ratio and CO<sub>2</sub> loading in the lean solvent suppressed aerosol emissions. In the pilot plant, the effects of four mitigation measures were evaluated, and it was found that dry bed and acid washing had better mitigation effects than did conventional water washing; amine emissions could be reduced to as low as 21 mg/Nm<sup>3</sup> PZ and 25 mg/Nm<sup>3</sup> AMP. This study provides a reference for the design and optimization of carbon-dioxide-capture systems, which can help to reduce the impact on the environment.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S277265682400085X/pdfft?md5=1cc9bb8194f28e2f8f31a48d520dff72&pid=1-s2.0-S277265682400085X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141993149","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}
Pub Date : 2024-08-16DOI: 10.1016/j.ccst.2024.100268
Direct air capture (DAC) represents an advanced negative carbon emission technology, with the key being high-performance CO2 adsorbents. First, this work carefully identifies CO2 physisorption and chemisorption by CaO/HcATP (CaO loaded on acid-modified attapulgite) as DAC adsorbent. The chemisorption of amorphous "CaO" plays a crucial role in both the adsorption capacity and rate, with contributions of 66.8 % and 50.85 %, respectively. The adsorption capacity of CaO/HcATP is only 212.4 ± 25.7 µmol/g via the simple CO2 physisorption and improved by 426.7 µmol/g owning to the chemisorption of amorphous CaO. Second, the concentration of silanol groups on CaO/HcATP plays a pivotal role in the adsorption process. The concentration of silanol groups decreases to 3.85 OH/nm2 after undergoing 30 cycles of adsorption-desorption. Then it increases to 9.54 OH/nm2 by adsorbing the moisture in the air, resulting in a recovered adsorption capacity of 90.7 %. Furthermore, the pseudo-first-order adsorption kinetics model effectively predicted the experimental results. Finally, the dual loop of CO2 capture and regeneration is summarized using the CaO/HcATP as DAC adsorbent. The amorphous "CaO" interacts with the surface silanol of HcATP, synergistically capturing CO2 in the form of "CaO···CO2", which reduces desorption energy consumption. The wetting property of HcATP contributes to the regeneration of CaO/HcATP. This work contributes to establishing fundamental principles for designing cost-effective DAC adsorbents.
{"title":"Design of alkali metal oxide adsorbent for direct air capture: Identification of physicochemical adsorption and analysis of regeneration mechanism","authors":"","doi":"10.1016/j.ccst.2024.100268","DOIUrl":"10.1016/j.ccst.2024.100268","url":null,"abstract":"<div><p>Direct air capture (DAC) represents an advanced negative carbon emission technology, with the key being high-performance CO<sub>2</sub> adsorbents. First, this work carefully identifies CO<sub>2</sub> physisorption and chemisorption by CaO/HcATP (CaO loaded on acid-modified attapulgite) as DAC adsorbent. The chemisorption of amorphous \"CaO\" plays a crucial role in both the adsorption capacity and rate, with contributions of 66.8 % and 50.85 %, respectively. The adsorption capacity of CaO/HcATP is only 212.4 ± 25.7 µmol/g via the simple CO<sub>2</sub> physisorption and improved by 426.7 µmol/g owning to the chemisorption of amorphous CaO. Second, the concentration of silanol groups on CaO/HcATP plays a pivotal role in the adsorption process. The concentration of silanol groups decreases to 3.85 OH/nm<sup>2</sup> after undergoing 30 cycles of adsorption-desorption. Then it increases to 9.54 OH/nm<sup>2</sup> by adsorbing the moisture in the air, resulting in a recovered adsorption capacity of 90.7 %. Furthermore, the pseudo-first-order adsorption kinetics model effectively predicted the experimental results. Finally, the dual loop of CO<sub>2</sub> capture and regeneration is summarized using the CaO/HcATP as DAC adsorbent. The amorphous \"CaO\" interacts with the surface silanol of HcATP, synergistically capturing CO<sub>2</sub> in the form of \"CaO···CO<sub>2</sub>\", which reduces desorption energy consumption. The wetting property of HcATP contributes to the regeneration of CaO/HcATP. This work contributes to establishing fundamental principles for designing cost-effective DAC adsorbents.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000800/pdfft?md5=a2a7fb403b63125fc7ec7aba6cc112e4&pid=1-s2.0-S2772656824000800-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141993148","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}
Pub Date : 2024-08-16DOI: 10.1016/j.ccst.2024.100276
Mixed-matrix membranes (MMMs) leverage the processability of polymers and selectivity of Metal-Organic Frameworks (MOFs). However, they still suffer from poor interfacial compatibility and limited scalability in preparation. In certain polymers, MOFs can bridge the pores within the polymer membrane, enhancing the CO2 adsorption and solubility properties, thus selectively boosting the CO2 permeability. In this study, high-performance MMMs were prepared using scalable CALF-20 in combination with PIM-1. MMMs with a 5% doping level achieved CO2 permeability up to 8003 barrer with 25% improvement in CO2/N2 selectivity. This enhancement was attributed to well-designed MMMs, where MOFs matched the abundant non-interconnecting pores in the PIM-1 membrane. This study represents a significant advancement towards scaling up the preparation of high-performance MOF-based MMMs for carbon capture applications.
{"title":"Scalable MOF-based mixed matrix membranes with enhanced permeation processes facilitate the scale application of membrane-based carbon capture technologies","authors":"","doi":"10.1016/j.ccst.2024.100276","DOIUrl":"10.1016/j.ccst.2024.100276","url":null,"abstract":"<div><p>Mixed-matrix membranes (MMMs) leverage the processability of polymers and selectivity of Metal-Organic Frameworks (MOFs). However, they still suffer from poor interfacial compatibility and limited scalability in preparation. In certain polymers, MOFs can bridge the pores within the polymer membrane, enhancing the CO<sub>2</sub> adsorption and solubility properties, thus selectively boosting the CO<sub>2</sub> permeability. In this study, high-performance MMMs were prepared using scalable CALF-20 in combination with PIM-1. MMMs with a 5% doping level achieved CO<sub>2</sub> permeability up to 8003 barrer with 25% improvement in CO<sub>2</sub>/N<sub>2</sub> selectivity. This enhancement was attributed to well-designed MMMs, where MOFs matched the abundant non-interconnecting pores in the PIM-1 membrane. This study represents a significant advancement towards scaling up the preparation of high-performance MOF-based MMMs for carbon capture applications.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000885/pdfft?md5=973267619c0e2fb3cba008394ac49789&pid=1-s2.0-S2772656824000885-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141992688","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}
Pub Date : 2024-08-14DOI: 10.1016/j.ccst.2024.100274
In this study, a novel composite was engineered by integrating Zr-MOF (NH2-UIO-66) with MXene layers through electrostatic self-assembly. Under simulated sunlight and at 80 °C, this composite material achieved nearly complete conversion of low-concentration atmospheric CO2 to CO and CH4 without additional sacrificial agents or alkaline absorption liquids, marking one of the few reports demonstrating near-complete reduction of low-concentration CO2 directly from the air. For high-concentration CO2 in industrial flue gas, the composite utilized residual heat at 80 °C without additional energy input, exhibiting excellent CO2 reduction efficiency with CO and CH4 production rates of 127 μmol·g-1·h-1 and 330 μmol·g-1·h-1, respectively, resulting in a total production rate 4.76 times higher than that in the air. Compared to most reports on thermocatalytic CO2 reduction (>300 °C), this material shows significant advantages below 100 °C. The performance improvement is attributed to the introduction of Zr-MOF, which provides additional active sites and reduces activation energy. Additionally, the localized surface plasmon resonance (LSPR) effect of MXene facilitates the migration of thermal charge carriers to Zr4+ sites within the MOF. Density Functional Theory (DFT) calculations validate these findings. Overall, Zr-MOF/MXene composite holds potential for reducing CO2 in air and industrial settings, advancing energy conversion and environmental management.
在这项研究中,通过静电自组装将 Zr-MOF (NH2-UIO-66) 与 MXene 层整合在一起,设计出了一种新型复合材料。在模拟太阳光和 80 °C 温度条件下,这种复合材料几乎完全将大气中的低浓度 CO2 转化为 CO 和 CH4,而无需额外的牺牲剂或碱性吸收液,这是少数几个直接从空气中几乎完全还原低浓度 CO2 的报告之一。对于工业烟道气中的高浓度 CO2,该复合材料利用 80 °C 的余热,无需额外的能量输入,表现出卓越的 CO2 还原效率,CO 和 CH4 生成率分别为 127 μmol-g-1-h-1 和 330 μmol-g-1-h-1,总生成率是空气中生成率的 4.76 倍。与大多数关于热催化二氧化碳还原(300 °C)的报道相比,这种材料在 100 °C以下具有显著优势。性能的提高归功于 Zr-MOF 的引入,它提供了额外的活性位点并降低了活化能。此外,MXene 的局部表面等离子体共振(LSPR)效应促进了热电荷载流子迁移到 MOF 中的 Zr4+ 位点。密度泛函理论(DFT)计算验证了这些发现。总之,Zr-MOF/MXene 复合材料有望减少空气和工业环境中的二氧化碳,促进能源转换和环境管理。
{"title":"Zr-MOF/MXene composite for enhanced photothermal catalytic CO2 reduction in atmospheric and industrial flue gas streams","authors":"","doi":"10.1016/j.ccst.2024.100274","DOIUrl":"10.1016/j.ccst.2024.100274","url":null,"abstract":"<div><p>In this study, a novel composite was engineered by integrating Zr-MOF (NH<sub>2</sub>-UIO-66) with MXene layers through electrostatic self-assembly. Under simulated sunlight and at 80 °C, this composite material achieved nearly complete conversion of low-concentration atmospheric CO<sub>2</sub> to CO and CH<sub>4</sub> without additional sacrificial agents or alkaline absorption liquids, marking one of the few reports demonstrating near-complete reduction of low-concentration CO<sub>2</sub> directly from the air. For high-concentration CO<sub>2</sub> in industrial flue gas, the composite utilized residual heat at 80 °C without additional energy input, exhibiting excellent CO<sub>2</sub> reduction efficiency with CO and CH4 production rates of 127 μmol·g<sup>-1</sup>·h<sup>-1</sup> and 330 μmol·g<sup>-1</sup>·h<sup>-1</sup>, respectively, resulting in a total production rate 4.76 times higher than that in the air. Compared to most reports on thermocatalytic CO<sub>2</sub> reduction (>300 °C), this material shows significant advantages below 100 °C. The performance improvement is attributed to the introduction of Zr-MOF, which provides additional active sites and reduces activation energy. Additionally, the localized surface plasmon resonance (LSPR) effect of MXene facilitates the migration of thermal charge carriers to Zr<sup>4+</sup> sites within the MOF. Density Functional Theory (DFT) calculations validate these findings. Overall, Zr-MOF/MXene composite holds potential for reducing CO<sub>2</sub> in air and industrial settings, advancing energy conversion and environmental management.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000861/pdfft?md5=11d2fcb0396247f5104b80e9a544ea9d&pid=1-s2.0-S2772656824000861-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141990421","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}
Pub Date : 2024-08-14DOI: 10.1016/j.ccst.2024.100275
The integrated CO2 capture and utilization employs chemical looping approach for suppressing the equilibrium limitations of traditional gas-solid catalytic reactions, enabling efficient conversion of dilute CO2 into high-value fuels with minimal energy consumption. However, the diminishing cyclic activity of dual-functional materials poses significant challenges to their industrial application. Herein, we tailored a series of magnesium-calcium materials, the influence of coordinated metals on the cyclic performance were quantitatively investigated. Notably, Fe2Ni2Ce2Mg5Ca20CO3 achieves a cumulative CO yield of 121.0 mmol/g over 15 cycles at 650°C, with a maximum CO yield of 8.3 mmol/g per cycle and 99.0% CO selectivity, and its CO2 capture capacity remains stable at 10.6 mmol/g over 37 adsorption/desorption cycles. Experimental results indicate that lattice phase separation is a fundamental mechanism underlying the decline in cyclic activity. The strategic incorporation of transition metal intermediates promotes the formation of dispersed metal-carbonate interfaces, providing surface hydrogenation sites and accelerating the lattice decomposition and reconstruction of CO3* within a dispersed lattice. This modification mitigates the adsorption/catalytic lattice phase separation, boosts metal migration and deoxygenation activity for cyclic nanoparticle construction. The findings offer valuable strategies for designing highly efficient and stable DFMs in CO2 capture and utilization.
二氧化碳捕获和综合利用采用化学循环方法来抑制传统气固催化反应的平衡限制,从而以最小的能耗将稀薄的二氧化碳高效转化为高价值燃料。然而,双功能材料的循环活性不断降低,给其工业应用带来了巨大挑战。在此,我们定制了一系列镁钙材料,定量研究了配位金属对其循环性能的影响。值得注意的是,Fe2Ni2Ce2Mg5Ca20CO3 在 650°C 下循环 15 次,累计 CO 产率达到 121.0 mmol/g,每次循环的最大 CO 产率为 8.3 mmol/g,CO 选择性达到 99.0%,并且在 37 次吸附/解吸循环中,其 CO2 捕获能力稳定在 10.6 mmol/g。实验结果表明,晶格相分离是导致循环活性下降的基本机制。过渡金属中间体的战略性加入促进了分散金属-碳酸盐界面的形成,提供了表面氢化位点,加速了分散晶格内 CO3* 的晶格分解和重构。这种改性减轻了吸附/催化晶格相分离,提高了金属迁移和脱氧活性,从而构建了循环纳米粒子。这些发现为在二氧化碳捕获和利用中设计高效稳定的 DFMs 提供了宝贵的策略。
{"title":"Suppressing cyclic deactivation of magnesium-calcium dual-functional materials via dispersed metal-carbonate interfaces for integrated CO2 capture and conversion","authors":"","doi":"10.1016/j.ccst.2024.100275","DOIUrl":"10.1016/j.ccst.2024.100275","url":null,"abstract":"<div><p>The integrated CO<sub>2</sub> capture and utilization employs chemical looping approach for suppressing the equilibrium limitations of traditional gas-solid catalytic reactions, enabling efficient conversion of dilute CO<sub>2</sub> into high-value fuels with minimal energy consumption. However, the diminishing cyclic activity of dual-functional materials poses significant challenges to their industrial application. Herein, we tailored a series of magnesium-calcium materials, the influence of coordinated metals on the cyclic performance were quantitatively investigated. Notably, Fe<sub>2</sub>Ni<sub>2</sub>Ce<sub>2</sub>Mg<sub>5</sub>Ca<sub>20</sub>CO<sub>3</sub> achieves a cumulative CO yield of 121.0 mmol/g over 15 cycles at 650°C, with a maximum CO yield of 8.3 mmol/g per cycle and 99.0% CO selectivity, and its CO<sub>2</sub> capture capacity remains stable at 10.6 mmol/g over 37 adsorption/desorption cycles. Experimental results indicate that lattice phase separation is a fundamental mechanism underlying the decline in cyclic activity. The strategic incorporation of transition metal intermediates promotes the formation of dispersed metal-carbonate interfaces, providing surface hydrogenation sites and accelerating the lattice decomposition and reconstruction of CO<sub>3</sub>* within a dispersed lattice. This modification mitigates the adsorption/catalytic lattice phase separation, boosts metal migration and deoxygenation activity for cyclic nanoparticle construction. The findings offer valuable strategies for designing highly efficient and stable DFMs in CO<sub>2</sub> capture and utilization.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000873/pdfft?md5=825fff2bf9fee572d40a1f50428a96f9&pid=1-s2.0-S2772656824000873-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141990585","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}
Pub Date : 2024-08-12DOI: 10.1016/j.ccst.2024.100266
The growth of coherently engineered porous bimetal (PBM) nanostructures shows great progress in electrochemical carbon dioxide (CO2) utilization. This is due to their remarkable catalytic and physicochemical merits that present an encouraging approach for CO2 conversion into valuable products (i.e., fuels and chemicals). Hence, this review presents recent advances in experimental, in-situ analysis and theoretical studies of PBM electrocatalysts, including PBM Cu-based and PBM Cu-free electrocatalysts, toward CO2 reduction reaction (CO2RR) and comprehend its fundamental mechanisms. Various synthesis strategies were utilized to construct PBM nanostructures with distinct compositions, morphology, and synergism for excellent CO2RR activity, stability and product selectivity. As corroborated by theoretical calculations that revealed beneficial electronic features and reaction routes with facile adsorption energies for reactant (CO2) and intermediate species on the various active sites of PBM nanostructures in easing the CO2RR. Future research efforts should establish robust framework for experimental, in-situ analysis, theoretical simulations and automated machine learning in developing next-generation electrochemical CO2 utilization technologies with PBM nanostructures. Finally, this study emphasizes the potential of PBM nanostructures for efficient electrochemical CO2 utilization and provides a pathway to sustainable and inexpensively viable carbon-neutrality.
{"title":"The advancement of porous bimetal nanostructures for electrochemical CO2 utilization to valuable products: Experimental and theoretical insights","authors":"","doi":"10.1016/j.ccst.2024.100266","DOIUrl":"10.1016/j.ccst.2024.100266","url":null,"abstract":"<div><p>The growth of coherently engineered porous bimetal (PBM) nanostructures shows great progress in electrochemical carbon dioxide (CO<sub>2</sub>) utilization. This is due to their remarkable catalytic and physicochemical merits that present an encouraging approach for CO<sub>2</sub> conversion into valuable products (i.e., fuels and chemicals). Hence, this review presents recent advances in experimental, <em>in-situ</em> analysis and theoretical studies of PBM electrocatalysts, including PBM Cu-based and PBM Cu-free electrocatalysts, toward CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) and comprehend its fundamental mechanisms. Various synthesis strategies were utilized to construct PBM nanostructures with distinct compositions, morphology, and synergism for excellent CO<sub>2</sub>RR activity, stability and product selectivity. As corroborated by theoretical calculations that revealed beneficial electronic features and reaction routes with facile adsorption energies for reactant (CO<sub>2</sub>) and intermediate species on the various active sites of PBM nanostructures in easing the CO<sub>2</sub>RR. Future research efforts should establish robust framework for experimental, <em>in-situ</em> analysis, theoretical simulations and automated machine learning in developing next-generation electrochemical CO<sub>2</sub> utilization technologies with PBM nanostructures. Finally, this study emphasizes the potential of PBM nanostructures for efficient electrochemical CO<sub>2</sub> utilization and provides a pathway to sustainable and inexpensively viable carbon-neutrality.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000782/pdfft?md5=5a085c56b579010b51ebd9502999ceb9&pid=1-s2.0-S2772656824000782-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141964627","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}
Pub Date : 2024-08-10DOI: 10.1016/j.ccst.2024.100263
As the global aviation industry faces increasing demands for carbon reduction, the need for sustainable aviation fuel (SAF) is also rising. SAF is similar to traditional kerosene-based aviation fuel but has significantly lower carbon emissions. This reduction is achieved through various routes, including carbon capture technologies and the use of biogenic-carbon feedstock, such as biomass, which contribute to overall emission reduction. However, as a new alternative fuel, SAF's application is limited due to a lack of awareness among countries and the absence of relevant regulations. This paper provides an overview of the current state of kerosene-based aviation fuel, the advantages of SAF, and analyzes the development potential and market for SAF, drawing on international regulatory experiences and mainstream production routes. Additionally, it organizes the certification systems and standards for SAF and discusses its techno-economic viability, technological maturity, and environmental benefits, particularly in terms of carbon emissions reduction. Finally, recommendations for the future development of SAF are provided to guide the aviation industry's green transition and the comprehensive market application of SAF.
随着全球航空业面临越来越多的减碳要求,对可持续航空燃料(SAF)的需求也在不断增加。可持续航空燃料与传统的煤油航空燃料类似,但碳排放量大大降低。这种降低是通过各种途径实现的,包括碳捕获技术和使用生物质等生物碳原料,这些都有助于总体减排。然而,作为一种新型替代燃料,由于各国缺乏认识和相关法规,SAF 的应用受到了限制。本文概述了煤油基航空燃料的现状、SAF 的优势,并借鉴国际监管经验和主流生产路线,分析了 SAF 的发展潜力和市场。此外,报告还整理了 SAF 的认证体系和标准,并讨论了其技术经济可行性、技术成熟度和环境效益,特别是在减少碳排放方面。最后,对 SAF 的未来发展提出了建议,以指导航空业的绿色转型和 SAF 的全面市场应用。
{"title":"Sustainable aviation fuels: Key opportunities and challenges in lowering carbon emissions for aviation industry","authors":"","doi":"10.1016/j.ccst.2024.100263","DOIUrl":"10.1016/j.ccst.2024.100263","url":null,"abstract":"<div><p>As the global aviation industry faces increasing demands for carbon reduction, the need for sustainable aviation fuel (SAF) is also rising. SAF is similar to traditional kerosene-based aviation fuel but has significantly lower carbon emissions. This reduction is achieved through various routes, including carbon capture technologies and the use of biogenic-carbon feedstock, such as biomass, which contribute to overall emission reduction. However, as a new alternative fuel, SAF's application is limited due to a lack of awareness among countries and the absence of relevant regulations. This paper provides an overview of the current state of kerosene-based aviation fuel, the advantages of SAF, and analyzes the development potential and market for SAF, drawing on international regulatory experiences and mainstream production routes. Additionally, it organizes the certification systems and standards for SAF and discusses its techno-economic viability, technological maturity, and environmental benefits, particularly in terms of carbon emissions reduction. Finally, recommendations for the future development of SAF are provided to guide the aviation industry's green transition and the comprehensive market application of SAF.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000757/pdfft?md5=32ebe0daca18cd1436037567e2ef35a9&pid=1-s2.0-S2772656824000757-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141963460","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}
Pub Date : 2024-08-08DOI: 10.1016/j.ccst.2024.100259
Excessive CO2 emissions present significant environmental and energy challenges, driving the need for effective strategies to reduce CO2. Integrated CO2 capture and utilization (ICCU) processes have drawn considerable attention by combing carbon capture and catalytic conversion in a unified process. The rational design of efficient dual-functional materials (DFMs) is key to achieving high-efficiency ICCU processes. Here, we synthesized a series of CaO-based DFMs with varying Ni loadings, in which the porous hollow CaO prepared by a sacrificial template method was employed as the adsorbent. The porous hollow structure are effectively to improve the diffusion of CO2 species and provide sufficient space for volume expansion after CO2 capture. The optimized conditions for adsorption and catalytic sites were determined to be at 550 °C with 5wt% Ni loading. Under these conditions, the adsorption capacity of 5 %Ni/CaO-P reached 7.02 mmol·g−1DFM, with a CH4 yield of 2.85 mmol·g−1DFM and a CH4 selectivity of 94.09 %. After 19 cycles, the adsorption capacity of 5 %Ni/CaO-P is maintained at 4.50 mmol·g−1DFM with a CH4 yield remaining stable at 0.50 mmol·g−1DFM due to the slight sintering of Ni species. Integrated CO2 capture and methanation offer a pathway for carbon recycling, emissions reduction, and sustainable development.
{"title":"Porous hollow Ni/CaO dual functional materials for integrated CO2 capture and methanation","authors":"","doi":"10.1016/j.ccst.2024.100259","DOIUrl":"10.1016/j.ccst.2024.100259","url":null,"abstract":"<div><p>Excessive CO<sub>2</sub> emissions present significant environmental and energy challenges, driving the need for effective strategies to reduce CO<sub>2</sub>. Integrated CO<sub>2</sub> capture and utilization (ICCU) processes have drawn considerable attention by combing carbon capture and catalytic conversion in a unified process. The rational design of efficient dual-functional materials (DFMs) is key to achieving high-efficiency ICCU processes. Here, we synthesized a series of CaO-based DFMs with varying Ni loadings, in which the porous hollow CaO prepared by a sacrificial template method was employed as the adsorbent. The porous hollow structure are effectively to improve the diffusion of CO<sub>2</sub> species and provide sufficient space for volume expansion after CO<sub>2</sub> capture. The optimized conditions for adsorption and catalytic sites were determined to be at 550 °C with 5wt% Ni loading. Under these conditions, the adsorption capacity of 5 %Ni/CaO-P reached 7.02 mmol·<em>g</em><sup>−1</sup> <sub>DFM</sub>, with a CH<sub>4</sub> yield of 2.85 mmol·<em>g</em><sup>−1</sup> <sub>DFM</sub> and a CH<sub>4</sub> selectivity of 94.09 %. After 19 cycles, the adsorption capacity of 5 %Ni/CaO-P is maintained at 4.50 mmol·<em>g</em><sup>−1</sup> <sub>DFM</sub> with a CH<sub>4</sub> yield remaining stable at 0.50 mmol·<em>g</em><sup>−1</sup> <sub>DFM</sub> due to the slight sintering of Ni species. Integrated CO<sub>2</sub> capture and methanation offer a pathway for carbon recycling, emissions reduction, and sustainable development.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S277265682400071X/pdfft?md5=70440aa0a214256731257d83e0c9a380&pid=1-s2.0-S277265682400071X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141963177","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}