INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Lei Wang,Zhiming Zhou,Yuanwu Hu,Zhenmin Cheng,Xiangchen Fang
A series of nanosheet MgO-based sorbents promoted by mixed-alkali-metal nitrate and carbonate were prepared by a simple precipitation–deposition method and applied to CO2 capture. The structural properties of these sorbents were characterized by various techniques, and their CO2 capture performance was evaluated using a thermogravimetric analyzer. Compared to the sorbent derived from commercial MgO, the nanosheet MgO-based sorbent had faster and higher CO2 uptake, because of its thin-sheet structure. Among various alkali-metal-salt-promoted nanosheet MgO, the sorbents promoted with mixed-alkali-metal nitrates (LiNO3 and KNO3) and carbonates (Na2CO3 and K2CO3) exhibited a high total CO2 uptake at a respectable rate. In particular, the sorbent with a MgO content of 73 wt % and a nitrate/carbonate molar ratio of 2 possessed the highest total CO2 uptake and the best cyclic stability, with a total uptake of 0.52 gCO2/gsorbent and MgO conversion of 65% after 20 cycles (60 min of absorption in 40% CO2/60% N2 at 350 °C, 15 min of regeneration in 100% N2 at 400 °C). Based on the structure–activity relationship of the sorbents, a possible mechanism consisting of three stages was presented for the CO2 absorption process, in which the dissolution of CO2 and carbonation in the molten nitrate played an important role.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 13
·5297-5304
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IF 3.269
Fengqin Yin,Peixuan Peng,Wenjie Mo,Shuixia Chen,Teng Xu
A porous amino resin melamine–formaldehyde (MF) with a high content of hydroxymethyl groups was prepared via the polycondensation of an excess of formaldehyde with melamine. Polyethylene imine (PEI) was then grafted onto the porous amino resin via a Mannich reaction between the active hydroxymethyl groups on the MF resin and the amino group on PEI to synthesize a solid amine adsorbent (MF-g-PEI). A large amount of hydroxymethyl groups were generated on the synthesized amino resin due to the excess formaldehyde used in the polycondensation reaction, which will provide abundant active sites to firmly combine with PEI and thus, enhance the stability of the MF-g-PEI adsorbent. The BET surface area and the pore volume of MF-g-PEI prepared using the optimal conditions were 460 m2 g−1 and 0.76 cm3 g−1, respectively. The CO2 adsorption capacity of MF-g-PEI, with a PEI loading of 11.35% can reach 1.32 mmol g−1 at 10 °C, while its amine utilization efficiency can reach up to 48.9%. The adsorbents also exhibited significantly improved adsorption kinetics and regeneration performance. This work provides a novel method that can achieve a promising solid amine adsorbent by directly grafting PEI onto porous material in the absence of an intermediate.
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Journal of CO2 Utilization
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2017
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IF 4.292
Yingjie Xu
Recently, chemical fixation of CO 2 catalyzed by protic ionic liquids (PILs) has been successfully achieved, suggesting that CO 2 absorption behavior plays an important role on CO 2 activation and transformation. For this reason, the influence of the alkalinity and physicochemical properties on CO 2 absorption behavior of four azole-based PILs, namely [DBNH][Pyr], [DBNH][Im], [DBUH][Pyr], and [DBUH][Im] was discussed in this work. The alkalinity of PILs was determined by potentiometric titration, and free space of PILs was evaluated by thermal expansion coefficient and refractive index. Solubility parameter of PILs was obtained from the activation energy for viscous flow. The results show that PILs with [Pyr] − exhibits stronger alkalinity and larger free space, which can help to improve CO 2 capture capacity. Whereas PILs with larger cation size [DBUH] + exerts higher viscosity, resulting in slower absorption rate of CO 2 . Furthermore, the CO 2 absorption capacity is inversely proportional to the solubility parameter of PILs. The absorption mechanism proved by FT-IR and 13 C NMR spectra indicates that [Pyr] − or [Im] − can react with CO 2 to form carbamate. Accordingly, considering the CO 2 capture capacity and absorption rate, [DBNH][Pyr] may be a good candidate for efficient CO 2 capture and activation with low enthalpy of absorption of −38.2 kJ mol −1 .
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Journal of Materials Chemistry A
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2017
·Vol. 5
·期 6
·2619-2628
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IF 8.867
Yuzhen Zhu,Zaixiang Xu,Wenya Jiang,Shuxian Zhong,Leihong Zhao,Song Bai
The utilization of a metal cocatalyst is a promising route to improve the solar-to-chemical conversion efficiency of semiconductor-based photocatalysts. The efficiency of the improvement is greatly dependent on the architectural structure of the metal cocatalysts, especially the catalytically active sites on the surface of the cocatalysts. In this article, Pd nanosheets with different sizes have been hybridized with TiO2 nanosheets to disclose how the edge of Pd cocatalysts influences the photocatalytic performance of TiO2–Pd hybrid structures in the reduction of CO2 to fuels. It was found that the highest photocatalytic activity was realized by small Pd nanosheets with the highest edge density on the TiO2 nanosheets. The reason is that the edges of the nanosheets act as the highly active sites for the CO2 reduction reaction. To further verify the edge-dependent photocatalytic performance, Pd nanorings were also deposited on the TiO2 nanosheets, which further improve the photocatalytic activity as compared with original nanosheets resulting from the additional edge sites exposed on the side of the hollow interior in the rings. This work underlines the importance in the edge engineering on the surface of cocatalysts in realizing high-performance photocatalytic applications.
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Nature Communications
·
2026
·
IF 18.1
Jiang Minwen,Liu Chang,Du Zhongyang,Tan Weiwei,Zheng Sihan,Liu Hai,Liu Pingying,Jiang Hejin,Lin Zhixing,Yao Changhong,Wang Fengzhong,Sun Peipei,Zhou Jiajing
The accelerating global energy demand, coupled with diminishing fossil fuel reserves and growing carbon emissions, underscores the urgent need for sustainable energy solutions. Autotrophic microalgae are promising cell factories for converting CO 2 into renewable biofuels. However, conventional microalgal biofuels typically depend on energy-intensive or nutrient-deficient regimes that suppress microalgal proliferation, resulting in a critical trade-off between biomass growth and lipid biosynthesis. Here, we report a separable living interface with microalgae (SLIM) platform that employs extracellular-matrix-mimicking hydrogel scaffolds to spatially organize microalgae and dynamically reconfigure their microenvironment, enabling spatiotemporal switching between biomass accumulation or lipid induction. The SLIM platform supports high-density growth of microalgae while facilitating precision substrate-driven metabolic regulation, enabling low-carbon operation and improved lipid production (8.89 g L −1 ). This work establishes an engineered living material that overcomes essential bottlenecks in microalgal biofuel production and offers a generalizable blueprint for biohybrid systems in advanced biomanufacturing.
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Journal of Energy Chemistry
·
2024
·
IF 14
Yuan Zhuang,Kaixuan Wei,Zhenxing Li,Hanzhang Gong,Jianan Deng,Haozhong Yuan,Haoyu Lian,Hao Zheng,Honghao Zhao,Xiao Zhang,Jian Liu
Designing the coordination environment of heteroatoms around metal sites and optimizing the electronic structure of diatomic metal sites remain significant challenges in achieving efficient CO 2 overall splitting. Herein, we report four configurations (Cu/Ni–N 4 C 2 , Cu/Ni–N 2 C 4 , Cu/Ni–N 2 C 3 and Cu/Ni–N 2 C 2 ) constructed by precise regulation of the coordination environment around bimetallic atoms. Cu/Ni–N 2 C 2 showed high performance in electrochemical CO 2 reduction (ECR) and water oxidation evolution reaction (OER). In the electrochemical CO 2 overall splitting reaction, it achieved a Faraday efficiency of CO (FE CO ) of 98.0% at a low cell voltage of −2.9 V, significantly higher than widely reported values. Moreover, the FE CO is above 90% over −2.7 to −4.1 V of cell voltages. Cu/Ni–N 2 C 2 achieved long-term ECR stability of 110 h at −100 mA cm −2 . Mechanism studies revealed that the change of coordination environment around the diatomic pairs moves the d-band center of the Ni atom closer to the Fermi level, thereby modulating the adsorption capacity of the catalysts to the reaction intermediates *COOH and *O. This work presents valuable insights into the rational design of diatomic catalysts and elucidates the intricate structure-performance relationship in advancing electrochemical CO 2 overall splitting technology and energy-conversion applications.
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Molecular Catalysis
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2024
·
IF 3.9
Tao Liu,Youcai Zhu,Yue Mu,Xindi Feng,Zhen Liu
CO 2 -based polyols have a unique terminal hydroxyl group structure that makes them suitable for the production of high-performance polyurethane foams. Zn-Co double metal cyanides (DMC) are an important class of catalysts for the copolymerization reaction of CO 2 with propylene oxide (PO). In the DMC-catalyzed CO 2 /PO copolymerization to produce CO 2 -based polyols, the crucial role of chain transfer agents (CTAs) is emphasized. In this work, a high-performance composite CTA (c-CTA) was successfully developed by investigating various dicarboxylic acids and polypropylene glycol (PPG-400) as CTAs. This system combines the high reaction rate of the DMC/PPG-400 system with the high CO 2 insertion rate of the DMC/sebacic acid (SA) system, achieving 2-3 times higher activity than that of single CTA (PPG-400 or SA), reaching 0.5 kg/g. The molecular characteristics of the CO 2 -based polyols synthesized by different DMC/CTAs systems were analyzed by FTIR and 1 H NMR. The reasons for the high catalytic activity of the DMC/c-CTA system were elucidated by analyzing the hydrogen bond distribution in each DMC/CTA systems. Overall, this work provides a theoretical guidance for the development of novel CO 2 -based materials with high industrial application value.
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Green Energy & Environment
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2024
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IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Fei Shi,Qinghua Li,Ye Yuan,Yi Yang,Xingzhong Cao,Menglong Sheng,Song Zhao,Zhi Wang
Interfacial polymerization (IP) has been received as an indispensable technology to fabricate thin-film composite (TFC) membranes for gas separation because of the simple and designable process. However, achieving the highly permeable polyamide (PA) TFC membrane for CO 2 capture via the IP technique remains challenging. Herein, a highly CO 2 -permeable PA TFC membrane was synthesized by the polycondensation of N, N-Bis [3-(methylamino) propyl]methylamine (BMAPAm) and trimesoyl chloride (TMC). The ultrathin (∼47 nm) PA TFC membrane featuring with high free volume exhibited excellent CO 2 permeance with moderate CO 2 /N 2 selectivity. The causes of this desired structure were systematically investigated from the aspects of monomer supply and molecular structure, in which the 3,3′-diamino-N-methyldipropylamine (DNMDAm) was used as a comparison. The results illustrated the underlying monomer-structure-performance relationships of IP-made membranes, demonstrating the solid potential of the IP technology specifically toward high-performance CO 2 capture membranes. Finally, a pilot-scale continuous membrane fabrication process was demonstrated.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 36
·15330-15337
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IF 3.5
Fangzheng Qi,Zengsheng Guo,Yuhan Zhang,Xue-Na Tang,Yiqiang Sun,Bo Xu,Guang-Ning Liu,Cuncheng Li
The stable contact of heterogeneous interfaces and the substantial exposure of active sites are crucial for enhancing the photocatalytic performance of semiconductor catalysts. However, most reported two-dimensional (2D)/2D CsPbBr3 and BiOCl heterostructures are fabricated using electrostatic self-assembly methods, which exhibit significant deficiencies in precise interface quality control and effective active site exposure. In this study, we fabricate a zero-dimensional (0D)/2D CsPbBr3/BiOCl heterojunction via a two-step calcination method, achieving an efficient direct S-scheme configuration. Optimizing interfacial contact and band alignment between CsPbBr3 quantum dots and BiOCl nanosheets enhances cross-plane charge transfer, promoting superior charge separation. This 0D/2D CsPbBr3/BiOCl heterojunction exhibits enhanced carrier mobility and high conversion rates without cocatalysts or sacrificial agents. The mechanism underlying the accelerated S-scheme charge transfer is comprehensively elucidated through a combination of analytical techniques and density functional theory (DFT) calculations. This study offers a novel approach for managing charge carrier segregation and mobility in CO2 reduction photocatalysts.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Guorui Liu,Guorui Ma,Haiqiang Mu,Jing Li,Feng Li,Min Zhu,Jin Zhang
Significant carrier recombination has severely limited the development of the most potential photoelectrocatalytic CO 2 reduction reaction (PEC-CO 2 RR). Herein, coral-like CuBi 2 O 4 -Bi 2 O 3 photocathodes are prepared using the strategy of the construction of heterojunction to improve the efficiency of carrier separation. As expected, its faradic efficiency of CO (FE CO ) at the lower potential (0.1 V vs. RHE) is 86.03 %, which is about 1.49 times higher than that of the original CuBi 2 O 4 film. The increased catalytic activity of CuBi 2 O 4 -Bi 2 O 3 can be attributed to the high surface area of the distinctive coral-like structure of Bi 2 O 3 , which enhances light absorption efficiency. Additionally, the higher degree of band bending in CuBi 2 O 4 -Bi 2 O 3 and the built-in electric field can speed up the transport rate of electrons, slow down the recombination of photogenerated electrons with holes and extend the lifetime of photogenerated electrons, allowing electrons to continuously participate in the reaction. This study proposes a novel strategy to optimize the efficiency of photoelectrocatalytic CO 2 reduction by CuBi 2 O 4 -based photocathodes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xinqi Zhang,Duoyong Zhang,Chen Zhang,Rongjie Ma,Xuancan Zhu,Liwei Wang
The capture of CO 2 from flue gas has emerged as the most effective technology for carbon reduction. The relatively low partial pressure of CO 2 in flue gas necessitates the development of CO 2 -selective adsorbents, which provide a direct pathway to obtaining pure CO 2 in one-step, thereby reducing energy consumption. Herein, an amino-rich deep eutectic solution (DES) is dispersed on the surface of formate ligand-removed MOF-808 using a self-assembly approach for post-combustion carbon capture. The high solubility of DES towards CO 2 enables the composite to effectively capture CO 2 , with MOF-808 serving as a porous gas storage tank. Material characterization confirms the loading of DES on the surface of MOF support while retaining its microporous structure. Owing to their unique CO 2 solution-diffusion mechanism, DES-modified adsorbents exhibit promising performance on CO 2 capacity, kinetics, CO 2 /N 2 selectivity, and isosteric heat. The optimized sample DES-2@MOF-808-FR demonstrates a notable CO 2 adsorption capacity of 4.16 mmol/g at 298 K and 1 bar. When tested with simulated flue gas (15 vol% CO 2 ), it maintains a working capacity of 2.86 mmol/g and a CO 2 /N 2 selectivity of 1184, surpassing most of existed materials. DES-2@MOF-808-FR can also retain its capacities after 10 adsorption/desorption cycles in simulated flue gas. This solution-based modification approach circumvents the challenges associated with precise structural control of the adsorbent, thereby facilitating potential industrial applications.
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