CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qiang Sun,Hongxia Gao,Teerawat Sema,Zhiwu Liang
High energy consumption during the carbon dioxide (CO 2 ) desorption process in amine-based CO 2 capture technology is a crucial hindrance to achieving carbon neutrality. HZSM-5 is one of the most widely reported solid acid catalysts used in primary amine regeneration. This work compared a series of HZSM-5 zeolites with different Si/Al ratios in terms of CO 2 desorption performance. To further enhance catalytic activity, hierarchical HZSM-5 was synthesized by the dealumination and desilication re-assembly method with different acid and alkali concentrations. The experimental results suggested that desilication by modification in sodium hydroxide resulted in a significant improvement of mesoporous surface area. The NaOH-0.4 catalyst could improve the amount of desorbed CO 2 by 40.3% and decrease the relative heat duty by 28.5%. And the cyclic tests revealed that catalytic activity was well preserved in the recycling process. Moreover, the structure and acidity of modification samples were characterized by X-Ray diffraction (XRD), Fourier transforms infrared (FT-IR), Nitrogen adsorption–desorption experiment, temperature programmed desorption of ammonia (NH 3 -TPD), Pyridine-adsorption infrared spectroscopy (Py-IR), and scanning electron microscopy (SEM). The characterization results suggested that the synergistic effect of larger mesoporous surface area and total acid sites was important to enhance catalytic CO 2 desorption performance. These results showed a new understanding of catalyst design for CO 2 capture technology by modifying the structure of the catalyst support.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Hui Wang,Hongyuan Chuai,Xiaoyi Chen,Jianlong Lin,Sheng Zhang,Xinbin Ma
Single-atom catalysts within M-N-C structures are efficient for electrochemical CO2 reduction. However, most of them are powdered and require a coating process to load on the electrode. Herein, we developed a facile approach to the synthesis of large-scale self-supported porous carbon nanofiber electrodes directly decorated with atomically dispersed nickel active sites using facile electrospinning, where poly(methyl methacrylate) was employed to tune well the distributions of pores located in carbon nanofibers. The above self-supported carbon nanofibers were applied as a gas diffusion electrode to achieve 94.3% CO Faraday efficiency and 170 mA cm–2 current density, which can be attributed to the effects of rich mesoporous structures favorable for adsorption and mass transfer of CO2 and single nickel catalysts effectively converting CO2 to CO. This work provides an efficient strategy to fabricate self-supported electrodes and may accelerate the progress toward industrial applications of single-atom catalysts in the field of CO2 electroreduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Lihua Han,Jian Mao,An-Quan Xie,Yunzheng Liang,Liangliang Zhu,Su Chen
Energy and freshwater, as natural and important strategic resources, are the lifeblood and basic security of economic and social development. Freshwater production consumes vast energy, and vice versa. It is rare and still a significant challenge in the rational design of implementation for efficient clean water and chemical fuel production via solar-thermal technology, reconciling the water-energy contradiction. Herein, we demonstrated a new double-stage solar catalytic membrane distillation (DSCMD) system, integrating photocatalyst into the photothermic electrospun film that is imparted with the water feeding, photothermic conversion and photocatalysis functions, which simultaneously realized the stable freshwater and enhanced clean fuels production. The photothermal/catalytic materials synergistically harvest photons for localized heat generation, which also acts on catalytically active sites to enhance the yield of vapor and CO, so as to maximize the utilization of solar energy. As a result, the overall freshwater collection rate of 1.45 kg m -2 h −1 with the solar-to-water efficiency of up to 90.6 % and enhanced CO evolution rate of 21.29 μmol g cat −1 h −1 from CO 2 photoreduction are achieved by more effective vapor transportation and latent heat recovery, superior to the traditional photothermal membrane distillation systems, providing an alternative opportunity for sustainably alleviating the freshwater and energy shortage.
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ENERGY
·
2022
·
IF 8.857
Kun Fu,Mingzhen Zheng,Dong Fu
The results of beaker experiments (Fu et al., 2021, 2022) showed that water-lean 2-ethylhexan-1-amine (EHA) + diglyme absorbent has more advantages than the commercial water-based ethanolamine (MEA) absorbent in terms of characteristics of carbon dioxide (CO 2 ) absorption and desorption. Verifying CO 2 capture characteristics in a tower facility is essential to absorbents development. In this work, a pilot packed tower was set up and the Dg16 type polypropylene step ring was taken as packing to test the capture efficiency and mass transfer performance of EHA + diglyme water-lean absorbent for low partial pressure CO 2 , and then the effects of gas-liquid ratio, CO 2 partial pressure and packing height on the capture performance were clarified. The results showed that the absorption of CO 2 by EHA + diglyme water-lean absorbent was dominated by liquid-phase mass transfer in the packed tower. Compared with aqueous 30 wt%MEA, the water-lean EHA + diglyme achieved much higher CO 2 capture efficiency and overall volumetric mass transfer coefficient. This work demonstrated the transition from water-free absorption to water-lean absorption under the existence of water vapor in flue gas . It can provide basic data for the design of the CO 2 capture process based on water-lean absorption in packed towers.
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CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Zhi-xiu Yang,Xiu Wen,Li-jing Gao,Jin Zhang,Rui-ping Wei,Xiao-mei Pan,Guo-min Xiao
The electrocatalytic carbon dioxide reduction provides a promising route to alleviate the greenhouse effect and energy crisis. We investigated the influencing factors that conversion of CO 2 to C 2 H 4 by preparing Cu 2 O nanoparticles (Cu 2 O-p, Cu 2 O-2p, and Cu 2 O-3p) with exposed different crystal facets, sizes, and grain boundaries. Impressively, the Cu 2 O-3p catalyst exhibits superior selectivity (57.8%) for C 2 H 4 generation due to its abundant {100} & {111} grain boundaries. The study demonstrated that rich grain boundaries have a significant effect on C C coupling for electrocatalysis CO 2 reduction, and offered a learnable route for high-efficient CO 2 reduction catalysts by regulating grain boundary.
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Small
·
2023
·Vol. 19
·期 19
·2208177
·
IF 13.3
Shuo Li,Yu-Jie Sun,Zhao-Xu Wang,Cheng-Gang Jin,Ming-Jie Yin,Quan-Fu An
Mixed matrix membranes (MMMs), conjugating the advantages of flexible processing-ability of polymers and high-speed mass transfer of porous fillers, are recognized as the next-generation high-performance CO 2 capture membranes for solving the current global climate challenge. However, controlling the crystallization of porous metal-organic frameworks (MOFs) and thus the close stacking of MOF nanocrystals in the confined polymer matrix is still undoable, which thus cannot fully utilize the superior transport attribute of MOF channels. In this study, the “confined swelling coupled solvent-controlled crystallization” strategy is employed for well-tailoring the in-situ crystallization of MOF nanocrystals, realizing rapid (<5 min) construction of defect-free freeway channels for CO 2 transportation in MMMs due to the close stacking of MOF nanocrystals. Consequently, the fabricated MMMs exhibit approximately fourfold enhancement in CO 2 permeability, i.e., 2490 Barrer with a CO 2 /N 2 selectivity of 37, distinctive antiplasticization merit, as well as long-term running stability, which is at top-tier level, enabling the large-scale manufacture of high-performance MMMs for gas separation.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 18
·e202203152
·
IF 4.3
Yan Long,Jie He,Hang Zhang,Yingkang Chen,Kang Liu,Junwei Fu,Hongmei Li,Li Zhu,Zhang Lin,Andrei Stefancu,Emiliano Cortes,Mingshan Zhu,Min Liu
Graphical Ag/Al 2 O 3 catalytic controllable synthesis of N-monomethylated amines by using CO 2 /H 2 as C 1 source has been demonstrated in a first example. The reactivity of methylated amines was reduced by the heterolytic dissociation of H 2 over the catalyst, and hence conversion of various amines to corresponding monomethylated amines was enabled with excellent selectivity. The selective synthesis of monomethylated amines with CO 2 is particularly challenging because the formation of tertiary amines is thermodynamically more favorable. Herein, a new strategy for the controllable synthesis of N-monomethylated amines from primary amines and CO 2 /H 2 is explored. First-principle calculations reveal that the dissociation of H 2 via an heterolytic route reduces the reactivity of methylated amines and thus inhibit successive methylation. In situ DRIFTS proves the process of formation and decomposition of ammonium salt by secondary amine reversible binding with H + on the Ag/Al 2 O 3 catalyst, thereby reducing its reactivity. Meanwhile, the energy barrier for the rate-determining step of monomethylation was much lower than that of overmethylation (0.34 eV vs. 0.58 eV) means amines monomethylation in preference to successive methylation. Under optimal reaction conditions, a variety of amines were converted to the corresponding monomethylated amines in good to excellent yields, and more than 90 % yield of product was obtained.
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AICHE JOURNAL
·
2023
·Vol. 69
·期 5
·e18025
·
IF 3.7
Chenxu Geng,Yuxiu Sun,Zhengqing Zhang,Zhihua Qiao,Chongli Zhong
Mixed matrix metal–organic framework (MOF) membranes show excellent application prospects in gas separation. However, their stability in various practical application scenarios is poor, especially under humid conditions. Herein, we encapsulated a hydrophobic ionic liquid (IL) into the cavity of MOFs, which effectively mitigated the competition between H 2 O and CO 2 in humid gas mixtures, leading to stable and high-performance gas separation. For this reason, the resulting membranes using polymer of intrinsic miroporosity-1 (PIM-1) as a polymer matrix show good CO 2 /N 2 separation performance and long-term test stability under humid environment. In particular, the 20 wt% IL-UiO/PIM-1 shows a high permeability of 13,778 Barrer and competitive CO 2 /N 2 separation factor of ~35.2, transcending the latest upper bound. Besides, the according membrane module exhibits slightly decreased CO 2 permeability and selectivity, promoting the application of self-supporting membranes. This work provides a reliable strategy for the rational design of MOF-based hybrid membranes under extreme conditions.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yu Liu,Zhichao Miao,Manfen Liang,Jie Zhang,Jinping Zhao,Leilei Xu,Jin Zhou,Shuping Zhuo
Electrocatalysis of CO 2 to CO is not only conducive to the artificial carbon cycle, but also green and efficient technology for producing chemicals. In consideration of the practical application, the novel strategy for large-scale preparation of catalyst has great potential to be developed. Herein, a facile one-step approach was developed for constructing a group of N -doping carbon-encapsulated metal catalysts (M@N C (M = Fe, Co, and Ni)) for CO 2 electroreduction to CO. In addition, the impact of metal on catalytic performance was detailedly researched. Specifically, the Ni@N C catalyst achieves an excessive CO Faraday efficiency (FE CO ) (>90 %) on a broad achievable potential window of − 0.67 V to − 0.97 V vs RHE in the H-type cell. The optimal catalyst attains a FE CO of 98 % at − 0.57 V vs RHE and an industrial-relevant current density of 430 mA cm −2 at − 1.07 V vs RHE in the flow cell. This work provides a facile way to fabricate catalyst on a large scale with preeminent performance for industrial CO 2 electroreduction to CO.
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Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 4
·1027-1040
·
IF 5.6
Ke Gao,Xianglei Liu,Qi Wang,Zhixing Jiang,Cheng Tian,Nan Sun,Yimin Xuan
Solar thermochemical CO2 splitting has emerged as a promising strategy for solar fuel production to alleviate climate change challenges and reduce the energy crisis. However, traditional redox materials still suffer from low CO production, poor cycle stability, high operating temperature, and large temperature swing, leading to low solar-to-fuel efficiency. Herein, Ce- and Al-doped SrMnO3 perovskites are proposed for high-performance solar thermochemical CO2 splitting within moderate temperature swing (1350/1100 °C). Sr0.6Ce0.4Mn0.8Al0.2O3 demonstrates a remarkable CO yield of 799.34 μmol g−1, which is ∼6.67 times as high as that of benchmark CeO2. Fast CO2 splitting kinetics of SCMA20 is demonstrated by the CO peak production rate enhanced by 142% compared with undoped SrMnO3. The proposed Sr0.6Ce0.4Mn0.8Al0.2O3 also exhibits excellent stability with no obvious deactivation or degradation over multiple cycles. The ultrahigh CO yield can be attributed to lower oxygen vacancy formation (3.65 eV) and migration energy (2.14 eV) as confirmed by DFT calculations, and the transformation of the first-order reaction (F1) to the second-order reaction (F2) compared to SrMnO3. This work provides a new path for high-performance solar thermochemical CO2 splitting with high CO production, fast reaction kinetics, good cycling stability, moderate temperature swing, and high solar absorptance.
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Solar RRL
·
2023
·Vol. 7
·期 7
·2201093
·
IF 7.9
Xiaohong Ma,Danyang Li,Jun Xie,Jian Qi,Huacheng Jin,Liuyang Bai,Hao Zhang,Feifei You,Fangli Yuan
The reduction of CO 2 to chemical fuel driven by solar energy can not only meet the growing demand for renewable energy, but also balance the carbon cycle in nature. However, the current photocatalysts have low CO 2 conversion due to their poor light capture ability, narrow light response range, and high recombination probability of photogenerated carriers. Herein, a heterogeneous photocatalyst of hollow structured ZnO/ZnS decorated with Pt nanoparticles is synthesized through the hydrothermal process and photodeposition method, showing excellent photocatalytic activity for CO 2 reduction in long-time stability and ≈100% CO selectivity, which can mainly contribute to natural enhanced light-capture ability of the hollow confined space due to multiple reflection and scattering of light in the cavity, thus improving separation efficiency of photogenerated charge carriers due to the type II junction constructed between ZnO and ZnS and the additional reaction active sites after decorating Pt nanoparticles in the surface of the hollow structure.
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Nature Nanotechnology
·
2023
·Vol. 18
·期 3
·299-306
·
IF 38.3
Wei Pengfei,Gao Dunfeng,Liu Tianfu,Li Hefei,Sang Jiaqi,Wang Chao,Cai Rui,Wang Guoxiong,Bao Xinhe
Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO 2 electrolysis performance. An alternative way is to use mixed CO/CO 2 feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO 2 co-electrolysis over CuO nanosheets in an alkaline membrane electrode assembly electrolyser. With increasing CO pressure in the feed, the major product gradually switches from ethylene to acetate, attributed to the increased CO coverage and local pH. Under optimized conditions, the Faradaic efficiency and partial current density of multicarbon products reach 90.0% and 3.1 A cm −2 , corresponding to a carbon selectivity of 100.0% and yield of 75.0%, outperforming thermocatalytic CO hydrogenation. The scale-up demonstration using an electrolyser stack achieves the highest ethylene formation rate of 457.5 ml min –1 at 150 A and acetate formation rate of 2.97 g min –1 at 250 A.
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