APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shaonan Zhang,Yuandong Yan,Qian Zheng,Shicheng Yan,Zhigang Zou
Carbon dioxide reduction reaction (CO 2 RR) on highly reactive frustrated Lewis pairs (FLPs) is a promising avenue for producing high-energy-density fuels from renewable energy. Exploring the effects of alkali metal ions on FLPs electrostatic field in neutral medium is a crucial knot for highly active FLP catalyst development. Here, leveraging the distinct electrochemical stability of In-OH and Bi-OH, we create stable Lewis pairs on the Bi 0.5 In 0.5 O y shell layer of Bi 0.5 In 0.5 O y @Bi 3 In 5 core-shell assembly with coordinatively unsaturated Bi-O Vs sites (Lewis acids) and In-OH (Lewis bases) to detect alkali metal ions effects. We find that K + is able to help electrochemically stable FLPs firstly capture and stabilize protons to protonate to Bi–H Lewis acid and In–OH 2 Lewis base due to their strong steric electrostatic field; then CO 2 is captured and activated by the protonated FLPs to produce formate with high selectivity. Whereas, Li + , Na + , and Cs + will inhibit CO 2 RR and promote the competing hydrogen evolution reaction due to Li + , Na + , and Cs + breaking steric electrostatic field of FLPs by inhibiting Bi-H formation. Our results verify that modulating electrostatic field of frustrated Lewis pairs by appropriate alkali cations is a promising catalyst design concept for highly selective CO 2 RR.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2025
·
IF 3.2
Shen Fumin,Yao Shunyang,Pei Yuanchao,Sun Rubin
The increasing levels of carbon dioxide (CO 2 ) emissions driven by industrial activities highlight the urgent need for the development of efficient and sustainable CO 2 capture technologies. Biomass-derived porous carbons have emerged as promising candidates for CO 2 adsorption due to their low cost, high surface area, and adjustable pore structure. In this study, hierarchically porous carbons (HPCs) were synthesized from waste acer truncatum wood through pre-carbonization and subsequent KOH activation. The synthesis conditions, including activation temperature and activating agent concentration, were optimized to precisely tailor the pore architecture. The resulting HPC exhibited excellent CO 2 adsorption capacities of 7.56 mmol·g⁻ 1 at 0 °C and 4.29 mmol·g⁻ 1 at 25 °C under ambient pressure. Notably, ultramicropores (< 0.7 nm) exhibited a dominant role in CO 2 capture at low pressures, while narrow micropores (< 1.0 nm) contributed significantly across a range of low-pressure conditions. The hierarchical pore structure enhanced CO 2 uptake at higher pressures. Furthermore, the material demonstrated exceptional CO 2 /N 2 selectivity, reaching up to 112 at 0.15 bar and 0 °C, along with good cyclic stability, highlighting its potential in post-combustion CO 2 capture. This work provides a sustainable strategy for converting waste biomass into high-value adsorbents, offering a solution that addresses both environmental concerns and economic feasibility.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Chen Feng,Haoxi Jiang,Lingtao Wang,Guochao Yang
CO 2 methanation is a critical process for converting CO 2 greenhouse gas into clean methane fuel, which holds significant strategic importance for environmental sustainability and energy sectors. Thermodynamic limitations demand low-temperature catalysts with enhanced low-temperature activity. This study employs solvent evaporation-induced self-assembly (EISA) to in-situ encapsulate Ni and Ce within SBA-15 molecular sieves. The approach significantly enhances low-temperature reactivity, achieving 67.5% CO 2 conversion and nearly 100% CH 4 selectivity at 300 °C, outperforming among Ni-based catalysts with silica carriers. Textural and electronic characterizations reveal that confinement effects of SBA-15 and electronic promotion of Ce synergistically strengthen the low temperature activity in methanation. This results in smaller Ni nanoparticles and an electron-rich Ni state, optimizing catalytic performance. Mechanistic analysis suggests that the Ce-modified Ni catalyst favors the formate pathway over the CO pathway, which supports the high methane selectivity and low carbon monoxide selectivity observed in this study.
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2025
·
IF 4.5
Bo Wen,Gaopeng Wang,Renze Xu,Chenglong Weng,Jintao Yang
With the growing global emphasis on environmental protection, supercritical CO 2 foaming technology for biodegradable materials such as polylactic acid (PLA), poly(butylene adipate-co-terephthalate) (PBAT), poly (butylene succinate) (PBS) and their blends has emerged as a research and application hotspot. However, the low melt strength and poor compatibility of these polymers often lead to low nucleation efficiency, cell wall rupture and coalescence, exhibiting inferior foaming performance. In this work, aiming to enhance the foamability of PLA and PLA/PBAT blends, a fluorinated chain extender, F-CE (GMA-co-DFHA-co-MMA), was designed and synthesized. Through the reactive melt blending, F-CE effectively enhanced the melt strength of PLA and interfacial adhesion between PLA and PBAT, leading to a significant improvement in foaming performance. Additionally, the fluorine groups in DFHA demonstrated high affinity for CO 2 , providing additional heterogeneous nucleation sites for bubble formation, thereby increasing both foam expansion ratio and cell density. Notably, the F-CE/PLA foam exhibited a cell diameter of ∼13.8 μm with an exceptionally high expansion ratio of ∼35. As a contrast, pristine PLA foam shows an expansion ratio of ∼30, but with large cell diameter (∼118 μm). Although PLA foam containing CE without fluorine (CE/PLA foam) exhibits small cells with an average cell diameter of ∼13.6 μm, the expansion ratio is low (∼23). In addition, F-CE also exhibits superior performance in improving the foamability of PLA/PBAT blends. This work presents a chain extender specifically engineered for foaming applications, which functions as a highly efficient foaming additive to holistically enhance the foaming performance of polymers.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jinshan Chen,Qiao Zeng,Shuangyou Bao,Fei Wang,Chi Wang,Kai Li,Yi Mei
Designing efficient and selective photocatalysts for CO 2 conversion under mild and practical conditions remains a significant challenge. This study aims to establish a sustainable strategy for constructing MOF-derived TiO 2 @TPA hybrids that enable efficient charge separation and selective CO 2 -to-CO conversion under low CO 2 concentrations without sacrificial agents. To achieve this, a TiO 2 @TPA hybrid material was synthesized via in-situ hydrothermal transformation of MIL-125(Ti) in water at 100 °C, without the use of organic solvents or high-temperature calcination. The resulting composite integrates TiO 2 nanocrystals with polymeric terephthalic acid (TPA) through Ti–O–C bonds, forming a stable interface that promotes ligand-to-metal charge transfer (LMCT). This interfacial structure enhances visible-light absorption and facilitates efficient charge separation. When applied to photocatalytic CO 2 reduction under low CO 2 concentrations (∼10 %), the TiO 2 @TPA hybrid achieved highly selective CO generation without the need for sacrificial agents or photosensitizers. In situ infrared spectroscopy and surface photovoltage analysis revealed the formation and stabilization of *COOH intermediates, elucidating the enhanced reaction pathway. This study demonstrates a scalable strategy for constructing MOF-derived hybrid photocatalysts and provides insights into interfacial design for selective CO 2 separation and conversion.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiaoyu Shi,Yang Yang,Xu Liu,Jingwen Wang,Fangming Jin
The current carbon capture and utilization (CCU) technologies suffer from energy-intensive processes due to conventional alkaline-based capture methods requiring significant energy input for regeneration and material cycling. In Earth’s carbonate weathering process within Karst systems, CO2 is sequestered and transformed through interaction with CaCO3. Inspired by this natural process, here, we propose an integrated CO2 capture–conversion strategy using geologically abundant carbonates as low-cost absorbents. We demonstrate that CO2 absorbed by carbonates can be efficiently hydrogenated in situ to formate in a one-pot system at 140 °C using a nonprecious cobalt–copper (CoCu) catalyst, achieving 21% yield of formate with diluted CO2 emissions (as low as 50 000 ppm, representative of typical industrial exhaust). Co facilitates the formation of a Cu+/Cu0 interfacial structure, leading to an enhancement of the hydrogenation efficiency. Density functional theory calculations show that the Cu+/Cu0 interface serves as the primary active site for H2 adsorption and activation to H*, which then promotes the reduction of bicarbonate (HCO3–) to formate. Furthermore, the interface between Co and Cu lowers the energy barrier for HCO3– adsorption, leading to its enhanced reduction by H*. This work offers a new pathway for simultaneous CO2 capture and catalytic conversion, advancing sustainable and energy-efficient CCU technologies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-16
·
IF 36.3
Peng Ting,Wang Yiqing,Dong Chung-Li,Nga Ta Thi Thuy,Wu Binglan,Wang Yiduo,Guan Qingqing,Zhang Wenjie,Shen Shaohua
BiOCl atomic layers (BOCNSs-i) were prepared by exfoliating hydrothermally synthesized BiOCl (BOCNSs) via ultrasonication in isopropanol for efficient photocatalytic CO 2 overall splitting to CO and O 2 .
The obtained BOCNSs-i photocatalyst exhibits a distinctly improved photocatalytic performance to stoichiometrically produce CO and O 2 at the ratio of 2:1, with the CO evolution rate reaching 134.8 µmol g −1 h −1 under simulated solar light (1.7 suns) and reaching 13.3 mmol g −1 h −1 under concentrated solar irradiation (34 suns).
With the thickness of BiOCl photocatalyst reducing to atomic layers, the charge carrier transfer and separation were enhanced by shortened transfer distance and the increased built-in electric field intensity, and electrons enriched Bi sites were exposed for activating CO 2 molecules.
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Pengcheng Ma,Wanshuang Zhou,Cong Yu,Zhuang Liu,Qiang Chen,Shi-Peng Sun,Xinbo Wang
Efficient CO 2 capture and separation are essential to enhance natural gas utilization and reduce coal-fired flue gas emissions, mitigating the climate change. Here, we introduce a novel acid-base dual-functional synergistic adsorption strategy by synthesizing a hypercrosslinked porous polymer (HCP-A-S) containing both amino and sulfonic acid functionalities. The material exhibits 0.34-nm ultramicropores and cooperative –NH 2 /–SO₃H groups that preferentially adsorb CO 2 , with CO 2 uptake and CO 2 /N 2 selectivity doubling that of the corresponding single-site HCP. DFT calculations reveal that the negatively charged amino groups and sulfonic acid moieties synergistically enhance CO 2 affinity through strong electrostatic and dipole–quadrupole interactions, facilitating highly selective capture. Dynamic breakthrough experiments confirm HCP-A-S's superior CO 2 /N 2 separation performance, high working capacity, and excellent recyclability. This dual-polar-site approach overcomes limitations of traditional single-site adsorbents and offers a cost-effective, scalable pathway to high-performance carbon capture materials.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mengdan Ma,Anning Zhou,Tao Hong,Xinyu Jia,Moxuan Liu
Metal-organic frameworks (MOFs) are promising materials for CO 2 adsorption and capture. The unique crystal structure and the open porous structure of MOFs are key factors affecting their CO 2 adsorption performance, but the precise tuning of MOF structures remains a challenge. Herein, we applied the Kamlet-Taft method to investigate the effect of solvent proton-supplying/accepting capaity (β/α parameters) on the structure and CO 2 adsorption performance of Mg-MOF-74 by tuning the reaction solvent polarity. It was found that the ratio of the nucleation rate/growth rate of Mg-MOF-74 could be effectively controlled by adjusting the β/α value of the solvent, realizing the regulation of the crystal structure and morphology of Mg-MOF-74. In addition, the size of solvent molecules played a crucial role in the pore size of Mg-MOF-74. Interestingly, the solvent molecules were competitively coordinated with ligands and participate in the growth of Mg-MOF-74 upon decreasing the β/α value. The crystal structure, morphology and pore size of Mg-MOF-74 could be precisely regulated by the β/α value and molecular size of the reaction solvent, and the highest performing Mg-MOF-74 exhibited a CO 2 adsorption capacity of 7.38 mmol/g.
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yonghong Wang,Xue Bai,Xinru Zhang,Jinping Li
Mixed matrix composite membranes (MMCMs) integrate the merits of inorganic and organic materials, but the tortuous transport passageways bring about large transfer mass resistance for gas transport. Herein, we prepared polyethylenimine-functionalized halloysite nanotubes (PEI-HNTs) by the electrostatic self-assembly of positively charged polyethylenimine and negatively charged halloysite nanotubes . Blending as-obtained PEI-HNTs with polyvinylamine (PVAm), MMCMs were prepared by casting above mixed solution on the top of ultrafiltration polysulfone (PSf) support. PEI-HNTs had good miscibility with PVAm due to hydrogen bonding . MMCMs (1 wt% PEI-HNTs loading) exhibited exceptional separation performance (CO 2 permeance: 179 GPU ; CO 2 /N 2 selectivity: 127.9), respectively, which were 1.4 and 2.3 times that of MMCMs embedding with 1 wt% HNTs. Noticeably, its value was beyond those of MMCMs incorporating with reported hollow tubular filler as well as other shape filler. This is due to the fact that PEI on the surfaces of HNTs provides a lot of amine carriers, which facilitate CO 2 transport. More importantly, the transport passageways are continuous, thus presumably reducing the CO 2 transfer resistance compared to other shape inorganic material filled-MMMs. Besides, resultant MMCMs revealed desirable stability for over 360 h, with a CO 2 /N 2 mixture as feed gas. Remarkably, it maintained superior gas separation performance (CO 2 permeance of 126 GPU; CO 2 /N 2 selectivity of 88.6) under the acidic conditions.
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 46
·23352-23359
·
IF 7.443
Wuxue Zhao,Sheng Han,Xiaodong Zhuang,Fan Zhang,Yiyong Mai,Xinliang Feng
A new series of B, N-containing cross-linked polymers (PPs-BN) were achieved via Sonogashira cross coupling. These polymers exhibit very high carbon yields of around 70–80% even at 800 °C, which allow them to be efficiently converted to B/N co-doped porous carbons after pyrolysis at high temperature under an inert atmosphere. The materials have been fully characterized by Fourier transform infrared spectroscopy, X-ray diffraction, thermogravimetric analyses, nitrogen sorption measurements and X-ray photoelectron spectroscopy, revealing their high contents of boron and nitrogen up to ∼3.21% and ∼5.72%, respectively, as well as porous structures with the largest specific surface area of 291 m2 g−1. Their CO2 capacities reached 3.25 mmol g−1 at 273 K under 1 atm. In addition, the very high selectivity for CO2/CH4 with a ratio of more than 5 : 1 at 298 K renders them applicable for gas separation and purification.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 94
·91557-91561
·
IF 3.289
Kechan Xia,Yifeng Yu,Yunqian Li,Shuhui Li,Yuying Wang,Guoxu Wang,Hongliang Zhang,Aibing Chen
Nitrogen-doped hollow carbon nanospheres (N-HCSs) have been synthesized by self-polymerization of dopamine on silica spheres using the modified Stöber method. The fabrication process uses dopamine as carbon and nitrogen source and tetraethyl orthosilicate as a structure-assisting agent. The particle sizes and shell thicknesses of the N-HCSs can be easily tuned in the range of 270–700 nm and 30–55 nm, respectively, by simply modifying the ethanol/water volume ratios. The surface areas of N-HCSs are in the range of 345–463 m2 g−1, and the total pore volumes are in the range of 0.34–0.52 cm3 g−1. The obtained N-HCSs have uniform mesoporous size of ∼4.0 nm, and high nitrogen loading content of 7.2 at%. Besides, the N-HCSs exhibit a considerable performance for CO2 capture with a capacity of 3.09 mmol g−1 at 25 °C and 1.0 bar and a good cycling stability.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）