Nature Communications
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2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Zheng Yue,Wang Huan,Liu Yan,Liu Peiyu,Zhu Baoli,Zheng Yanning,Li Jinhua,Chistoserdova Ludmila,Ren Zhiyong Jason,Zhao Feng
The chemical transformations of methane (CH 4 ) and carbon dioxide (CO 2 ) greenhouse gases typically have high energy barriers. Here we present an approach of strategic coupling of CH 4 oxidation and CO 2 reduction in a switched microbial process governed by redox cycling of iron minerals under temperate conditions. The presence of iron minerals leads to an obvious enhancement of carbon fixation, with the minerals acting as the electron acceptor for CH 4 oxidation and the electron donor for CO 2 reduction, facilitated by changes in the mineral structure. The electron flow between the two functionally active microbial consortia is tracked through electrochemistry, and the energy metabolism in these consortia is predicted at the genetic level. This study offers a promising strategy for the removal of CH 4 and CO 2 in the natural environment and proposes an engineering technique for the utilization of major greenhouse gases.
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ACS Applied Nano Materials
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2025
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IF 5.5
Qiangshuai Wang,Sengui Liang,Jinshuo Liu,Yuanyuan Xie,Qi Pang,Zhao-Qing Liu,Yibo Chen
Photocatalytic conversion of carbon dioxide (CO2) to carbon-based fuels is a promising approach to alleviating environmental and energy problems. Therefore, designing photocatalysts with morphological structures that favor gas–solid reactions and exhibit exceptional catalytic efficiencies is strongly demanded. In this work, a porous-framed heterostructure, constructed by anchoring Cs4PbBr6 perovskite nanocrystals on MnO2 hollow spheres, exhibits a 1.8-fold enhancement in the total electron consumption rate (95.3 μmol g–1 h–1) for CO2 photoreduction compared to the original Cs4PbBr6 nanocrystals. Detailed optoelectronic characterizations and theoretical calculations demonstrate that the electronic interactions in the heterointerface trigger disproportionation of Mn and help to expose active Mn sites that attract electrons, thus improving the CO2 activation and the following hydrogenation step to produce COOH*. The open and through porous structure also contributes to the enhanced reaction rate by accelerating mass transfer during the photoreduction reaction. This study provides valuable insights for the development of efficient catalysts for CO2 photoreduction in gas–solid reactions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Luming Qi,Zhenyang Rong,Yeyang Ni,Linlin Zhang,Zhe Zhou,Qing Liu,Jihai Tang,Mifen Cui,Xu Qiao
The development of highly stable structured solid amine adsorbent is crucial for the large-scale deployment of CO 2 capture systems. Here, we report a structured solid amine adsorbent using the solid-liquid hybrid wrapping method, wherein a suspension of tetraethylenepentamine (TEPA) and ZSM-22 support is encapsulated within a calcium alginate film through freeze-drying. The textural properties of the structured adsorbents (SA@S/T X ) were investigated using scanning electron microscopy, N 2 adsorption-desorption, Fourier transform infrared spectroscopy, and thermal gravimetric analyzer. The CO 2 adsorption capacity of SA@S/T X displayed an initial increase followed by a decrease with increasing TEPA loading, and the adsorption rate exhibited a similar trend according to the pseudo-first-order model. The maximum adsorption capacity and adsorption rate ( k ) were observed to be 2.22 mmol/g and 0.98 min −1 (under conditions of pure CO 2 , 1 atm and 25 °C), respectively, at a TEPA content of 0.5. In addition, SA@S/T X exhibited good regeneration stability with a low loss in capacity of 10.8 % during 30 cycle of CO 2 adsorption–desorption tests, and high thermal stability with a low amine loss of 2.0 % under conditions of 100 °C and 12 h. These results demonstrate that the solid–liquid hybrid wrapping method effectively shapes the powdered adsorbent while significantly reducing TEPA volatilization, offering a possibility for the industrial applications of solid amine adsorbents.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Han Zhang,Tao Yan,Zhikun Liu,Wenjing Xu,Yingying Cheng,Peng Kang
Electrocatalytic reduction of CO2 is an effective way to solve environmental issues. In this article, we report an inexpensive, readily available zinc oxide catalyst (TEA-ZnO) functionalized using alkanolamine, which is highly active and selective for the reduction of CO2 to generate CO at elevated temperatures. Triethanolamine-modified zinc oxide (TEA-ZnO) shows ca. 88.8% CO Faradaic efficiency at −0.84 V vs RHE. The amine groups of triethanolamine could increase the adsorption capacity of CO2, expose more CO2-specific active sites, and mitigate the high-temperature decrease of CO2 solubility, which enables TEA-ZnO to maintain high CO2 selectivity in the temperature range of 0–60 °C.
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Small
·
2025
·
IF 12.1
Xinyi Sun,Zhang Wen,Yiwen Liu,Min Zhang,Wei Li,Chuanchao Sheng,Sixie Yang,Haoshen Zhou,Ping He
Environmental-friendly aqueous Zn−CO 2 batteries present bifunctional potentials of achieving carbon neutrality and energy storage. Nonetheless, anode corrosions derived from H 2 O molecules and high risks of volatilization and leakage hinder the advancement of Zn−CO 2 batteries. In this work, polyvinyl alcohol (PVA)-based hydrogel electrolyte with fast ion diffusion kinetics, high mechanical strength, and flexibility is developed to replace liquid electrolyte. Since hydroxyl radicals in the polymer chain can interact with H 2 O and Zn 2+ , electrode corrosion from free H 2 O and active H 2 O around Zn 2+ is significantly inhibited, facilitating the uniform deposition of Zn 2+ cations. The introduction of an ionic liquid plasticizer further enhances the interaction between Zn 2+ and polymer backbone, as well as amorphous extent of the electrolyte. The hydrogel electrolyte possesses adequate self-healing ability, whose ionic conductivity reaches 7.95 × 10 −3 S cm −1 . The symmetric Zn metal batteries containing the electrolyte remain steady for >2000 h under different current densities. Furthermore, the Zn−CO 2 battery based on Ru nanoparticles cathode and hydrogel electrolyte realizes a discharge capacity of 6028 mAh g −1 and stable cyclicity for 90 times. The reaction path of hydrogel electrolyte-based Zn−CO 2 battery is that CO 2 is reduced to ZnCO 3 and C species followed by reversible decomposition of discharge products on recharge.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yanpeng Chen,Rongshu Zhu,Guanyu Chen,Minghu Zhao,Min Ju,Rongming Cai,Jinqiang Gao,Mei Hong,Shihe Yang
Synthesis of small-pore chabazite (CHA) zeolites in the absence of organic structure-directing agents (OSDA) has been proven difficult. A judicious mixed cation approach recently reported could expand the design space of CHA formation. In a seemingly opposite direction, we herein report an anion tuning approach for controlling the zeolite polymorphism in an OSDA-free system that effectively promotes hierarchical CHA formation in a competitive growth with MER. Phenoxide media, utilizing mild in-situ nucleophilic etching in cooperation with zeolite framework growth, allow beneficial kinetic control to facilitate CHA nucleation. Operando analyses reveal the crucial role of stabilized dimeric aluminate species as a key intermediate for CHA phase selection. The phenol-mediated CHA zeolites exhibit almost perfect 9 molecules per unit cell CO 2 uptake capacity and no CH 4 adsorption. This work offers an anion tuning strategy for controlling zeolite polymorphism as a supplement to the current phase-selection toolbox that utilizes mixed inorganic cations.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Tengfei Zhang,Peng Zheng,Jiajian Gao,Zhennan Han,Fangna Gu,Wenqing Xu,Fang Wang,Tingyu Zhu,Guangwen Xu,Ziyi Zhong,Fabing Su
Redispersing bimetallic active nanoparticles in a heterogeneous catalyst can significantly improve metal utilization and catalytic performance, but it is very challenging. In this work, we report a feasible method to redisperse large bimetallic NiRu particles (30–40 nm) on the CeO 2 support into small alloyed NiRu nanoparticles (3–5 nm) in an Ar gas atmosphere (NiRu/CeO 2 -Ar). During the high-temperature treatment, Ru metal in big bimetallic NiRu particles migrated to the surface of small alloyed nanoparticles because of the metal-phase separation, forming more Ni−Ru metal interfaces. As a result, NiRu/CeO 2 -Ar showed much better catalytic performance in CO 2 methanation than the pristine catalyst (NiRu/CeO 2 ) and the catalysts treated in air, H 2 , and reactant gases, respectively. Experimental and theoretical calculation results reveal that the newly generated Ni−Ru metal interfaces are conducive to the adsorption of CO 2 and further direct dissociation into CO*, thus enhancing the catalytic performance. This work provides a reliable strategy to redisperse bimetallic NiRu nanoparticles into small ones with more intermetallic interfaces.
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Journal of CO2 Utilization
·
2024
·
IF 7.2
Xiaomeng Deng,Wensheng Wei,Zizhen Yan,Zhanguo Zhang,Yuxin Wang,Guangwen Xu,Jianjun Guo,Jinggang Zhao,Lei Shi
A meaningful and practical phenomenon was observed and investigated, about which a synthesized (2-hydroxyethyl) triethylammonium bromide (NEt 3 (HE)Br) was used for catalytic cycloaddition of PO (propylene oxide) and CO 2 (carbon dioxide) in a homogeneous state, and then separated from the reaction system in a heterogeneous state. The target products were first reported as additives to regulate the distribution of reactants and carbon dioxide (CO 2 ) in the gas-liquid phase, as well as to facilitate the dissolution of NEt 3 (HE)Br. Under the optimal conditions of 0.2 mol% NEt 3 (HE)Br dosage, the PC yield (98.71 %) and TOF value (22.54 h −1 ) reached are significantly higher than the case of without PC addition. Besides, NEt 3 (HE)Br exhibited impressive stability after five catalytic cycles. The catalytic performances of different additives (i.e., alcohols, cyclic carbonate, amides, sulfones, petroleum ether, straight-chain carbonate and oxalate) were investigated, and their promotional effects and mechanisms were systematically elucidated. The transition behavior of dissolution-catalysis-precipitation process and intrinsic promoting mechanism of NEt 3 (HE)Br gave an efficient idea for a homogeneous catalytic reaction and heterogeneous separation of the catalyst. Meanwhile, this work provides an important theoretical and practical basis for efficient and facile catalyst synthesis and the corresponding reaction system design.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Xiaofan Yang,Siyu Yi,Zhaolong Wang,Zhongqiu Wu,Ying Zhang,Junjie Yuan,Haibo Wang,Xiaojie She,Hui Xu
Electrocatalytic CO2 Reduction Reaction (ECO2RR) driven by renewable energy, which could convert CO2 into fuels or value-added chemicals, has become an effective approach to address environmental issues and the energy crisis. However, due to the low selectivity, the inferior activity, and unmanageable reconstruction of catalysts, the path of ECO2RR remains a significant challenge. In this study, a series of electrocatalysts composed of copper–lanthanum nanoparticles dispersed within a nitrogen-doped carbon framework (LaCu@NCF-x, where x represents the abbreviation of calcination temperatures) were synthesized by calcining the mixture of polymers and metal ions, in which thermal control is the key to the catalyst preparation process. Phase and morphological characterizations reveal that the degree of carbonization and the accessibility of active sites were modulated by the temperature of calcination. The study highlights the importance of the synergistic and confinement effects of the encapsulating carbon layer, which not only provides a favorable matrix for the nanoparticles but also mitigates the reconstruction of electrocatalysts, thereby significantly enhancing its performance in CH4 production during ECO2RR. In particular, the LaCu@NCF-3 catalyst demonstrates the maximum Faraday efficiency (FE) of CH4 up to 64.6% at −1.177 V vs RHE and superior stability. Moreover, it also maintains a high selectivity (FECH4 ≥ 60%) over the wide potential range from −0.977 V to −1.577 V vs RHE. This study provides a novel approach to the fabrication of efficient and stable Cu-based electrocatalyst for ECO2RR to CH4.
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JOURNAL OF POLYMER RESEARCH
·
2025
·Vol. 32
·期 9
·1-10
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IF 2.8
Lun Ziming,Song Lina,Ai Jiaoyan,Zhong Tulian,Xian Wenqi,Liu Baohua
A series of CO 2 -based UV cured polyurethane acrylate with good flexibility and mechanical strength were prepared using polycarbonate diol (PECD), diphenylmethane diisocyanate (MDI), hydroxyethyl acrylate (HEA), and tetrahydrofuran acrylate (THFA) as raw materials. Simultaneously compared with traditional polyester (PCLD)-based and polyether (PPG)-based UV cured polyurethane acrylates. By analyzing the infrared spectra of prepolymer and PECD-PUA, the generation of characteristic absorption peaks indicates the successful synthesis of PECD-PUA. In addition, compared with the uncured film, the carbon carbon double bond absorption peak (810 cm -1 ) of the cured film disappeared, indicating that the double bond had undergone a reaction. The mechanical properties, hardness, water contact angle, and solvent absorption properties of UV-cured polyurethane were studied. The results show that the CO 2 -based material PECD has excellent properties, the tensile strength can reach 9.83 MPa, and the elongation of break reach 82.92% and the cured UV-PECD-PU film has high hardness (pencil hardness: HB) All cured films exhibited excellent thermal stability (more than 250 ℃) through TGA analysis. This paper synthesized environmentally friendly CO 2 -based photopolymerization polyurethane, providing direction for the resource utilization of carbon dioxide-based materials.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Mengjun,Jia Jun,Xia Jing,Peng Chun-Kuo,He Jinxin,Qiu Yueming,He Yuting,Gao Le,Xue Fei,Lin Yan-Gu,Zhan Guowu,Guo Yuzheng,Huang Xiaoqing,Xu Yong
Carbon dioxide (CO 2 ) conversion to liquid fuels has attracted great attention due to the current environmental concerns and energy crisis. However, the selective conversion of CO 2 to target liquids is formidably challenging due to the chemical inertness of CO 2 . We theoretically and experimentally confirm that the bending of Pd−Pd bond can breaks the asymmetric potential well and facilitate CO 2 adsorption. We have successfully synthesized a new class of Pd nanoneedles via a “close edges and open corners” process, with a magic angle of 60 o between the main trunk and branch, and realized the selective CO 2 hydrogenation to formic acid (HCOOH) at room temperature in water. Impressively, a HCOOH productivity of ~250 mmol g −1 in 100 h while maintaining HCOOH selectivity over 99%. This work bridges nanostructure design and catalytic application, which may open a new avenue for selective CO 2 conversion in an elegant manner.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Liqing Chen,Kejia Fan,Luting Yan,Jingfa Yang
Global economic and technological advancements have led to a significant surge in CO 2 emissions, posing severe environmental challenges. This study explores the photocatalytic reduction of CO 2 using a high-entropy fluorite oxide (HEFO), (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Ca 0.2 )O 2-δ , synthesized via solid-state reactions. XRD, SEM, and XPS analyses confirmed a single-phase fluorite structure and revealed excellent light absorption (250–400 nm) with a 2.6 eV bandgap. Photocatalytic CO 2 reduction experiments demonstrated the superior performance of fine particles (72 % CO 2 conversion, 12.01 μmol h −1 g −1 methane generation, 61.2 % selectivity) compared to that of coarse one. This enhanced activity was attributed to a higher oxygen vacancy concentration, which optimized the surface electronic structure, increased the number of active sites, and improved CO 2 adsorption and activation. This study highlights the potential of HEFOs for renewable fuel production via CO 2 photoreduction.
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