JOURNAL OF MATERIALS SCIENCE
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2025
·Vol. 60
·期 48
·25741-25761
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IF 3.9
Gao Ningning,Pan Yucheng,Huang Wei,Xin Qingping,Zhang Min,Wu Jiaxin,Wu Dengdi,Wang Mengke,Ding Xiaoli,Lin Ligang,Zhang Yuzhong
Due to its benefits of low energy consumption, minimal environmental pollution, and simple operation, membrane technology is considered a carbon capture technology with extensive application possibilities. In this study, the ultraviolet cross-linking method is used to inhibit crystallization of polymers with a molecular weight of less than 1500 and enable polyethylene oxide (PEO) to form a rubbery polymer matrix. This approach avoids membrane separation defects and low CO 2 solubility caused by high crystallinity. The hydroxyl-rich surface of layered double hydroxide (LDH) is used to provide the CO 2 -philic site in the form of “docking station-like” by introducing amino groups with a strong affinity for CO 2 , and forming a dual facilitated transport channel through the nanosheet interlayer channel and the presence of bound water to strengthen the reaction mechanism of the membrane. Based on the coupling of solubility-diffusion and facilitated transport mechanisms, the optimal separation performance is achieved when the NH 2 -PDA-LDH doping is 0.4 wt%, with a CO 2 permeability of 572.4 Barrer and a selectivity of up to 60.5. The interlayer fast transport channels result in a maximum permeability of 3982 Barrer in the wet state. Graphical
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 13.2
Huiyuan Cheng,Jingwei Hu,Shaoke Bu,Yushuang Shi,Guangping Lei
The escalating atmospheric concentration of CO 2 has intensified the demand for efficient carbon capture technologies. Here, an innovative composite adsorbent, Cu-Salophen@Cu-BTC, was successfully synthesized via an in-situ encapsulation strategy to enhance the selective adsorption of CO 2 from CO 2 /N 2 mixture. The incorporation of Cu-Salophen into the Cu-BTC framework was confirmed through XRD, ICP-OES, and FT-IR analyses. The composite exhibited a notable improvement in CO 2 uptake capacity, reaching 8.14 mmol g −1 (273 K) and 4.63 mmol g −1 (298 K) at 100 kPa, representing increases of 11.81% and 12.11%, respectively, compared to pristine Cu-BTC. Moreover, the CO 2 /N 2 separation performance was enhanced by 23.44% (273 K) and 36.06% (298 K). GCMC simulations revealed that the superior performance arises from the synergistic effects of additional adsorption affinities of CO 2 and real-time pore size regulation enabled by the mobile Cu-Salophen molecules. The composite also demonstrated excellent recyclability and improved water stability, underscoring its potential for industrial post-combustion CO 2 capture.
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Journal of CO2 Utilization
·
2017
·
IF 4.292
Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao
An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2 + H 2 → CO + H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.
研究领域:
绿色化学
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有机合成
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催化化学
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环境友好工艺
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工业化学
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RENEWABLE ENERGY
·
2026
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IF 9.1
Huage Lin,Weiyan Su,Yihan Tang,Jiaxiang Zong,Guangyu Wu,Weinan Xing
The scalable synthesis of green chemical fuels via artificial photosynthesis represents a cornerstone strategy for buffering intermittent renewable energy and advancing global carbon neutrality. However, the practical engineering deployment of this technology is severely constrained by suboptimal solar-to-fuel conversion efficiencies at the catalytic interface. Herein, a tubular S-scheme Co 2 (OH)PO 4 @CN (CoHP@CN) heterojunction was fabricated via a pre-coordination-mediated in-situ growth strategy to facilitate solar energy harvesting. Characterizations reveal that a directional internal electric field (IEF) drives an S-scheme charge pathway, significantly reducing transfer resistance while preserving strong redox capabilities. Benefiting from these kinetic features, the heterojunction delivers exceptional solar fuel production performance, achieving a CO yield of 383.40 μmol g −1 (over 4 h) and H 2 evolution of 4657.40 μmol g −1 (within 2 h). This study underscores the power of precise interface engineering in modulating charge dynamics, offering practical insights for scalable solar-to-chemical energy storage and renewable energy deployment.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 32
·43974-43984
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IF 7.8
Zhang Chuyi,Sun Zhi,Kong Weiqian,Wu Wenzhuo,Zheng Xiaoli,Xu Qun
The enhancement of photocatalytic efficiency is limited by exciton dynamics, where photogenerated electrons and holes rapidly recombine due to strong Coulomb attraction. The manipulation of electron spin, involving the control of electron spin and spin states, has emerged as a promising strategy to improve photocatalytic performance via spin-polarization-facilitated charge separation. In this work, we demonstrate a spin-polarization effect achieved by treating ZnSn(OH) 6 (ZHS) with supercritical CO 2 (SC CO 2 ), which accelerates exciton dissociation and spin-dependent electron migration, thereby enhancing the efficiency of photocatalytic CO 2 reduction to CO. Mechanistic investigations reveal that SC CO 2 treatment induces oxygen vacancies in ZHS, generates spin-polarized electrons, and selectively exposes highly active {111} crystal facets. Experimentally, it reveals that the oxygen vacancies, together with adjacent hydroxyl groups, construct frustrated Lewis pairs (FLPs). Through enhanced quantum spin exchange interactions (QSEIs), the recombination of photogenerated charge carriers is significantly suppressed, and then their lifetime is prolonged, and CO 2 adsorption and activation are simultaneously enhanced. It was found that, under treatment at 16 MPa of SC CO 2 , the CO production rate of ZHS reaches 144.82 μmol·g –1 ·h –1 , which is 29.37 times that of the untreated sample. Therefore, this study demonstrates that manipulating spin-polarized electrons in photocatalytic semiconductors is an effective strategy to boost CO 2 RR efficiency, offering new insights for the design of efficient spin-dependent photocatalysts toward solar energy conversion.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Si Liu,Zixuan Xu,Qun Liao,Xingxing Zheng,Xionghui Fu,Yuanming Zhang,Yi Zhu
Co₃O₄/TiO₂ achieves a CH₄ yield of 34.8 μmol g −1 h −1 with 82.4% selectivity. • Ti–O–Co bonds serve as charge transfer channels in Co₃O₄/TiO₂. • Co 2+ /Co 3+ redox couples stabilize *CO intermediates and facilitate PCET. • Electron transfer promotes Co electron enrichment for *CO stabilization. • Synergistic electron transfer and proton supply promote selective CO₂ methanation. Value-added conversion of CO 2 using solar energy is a sustainable strategy to address the energy crisis and environmental issues simultaneously. In this work, Co 3 O 4 /TiO 2 composite photocatalysts were successfully prepared by a hydrothermal method. The optimized Co 3 O 4 /TiO 2 achieves a CH 4 yield of 34.8 μmol·g −1 ·h −1 with 82.4% selectivity. The enhanced catalytic activity is ascribed to interfacial Ti-O-Co bonds that facilitate electron transfer toward Co sites, thereby modulating the Co 2+ /Co 3+ electronic environment and creating relatively electron-rich Co sites for *CO stabilization, while the Co 3 O 4 component facilitates the proton-coupled electron transfer (PCET) process toward CH 4 formation. This study provides a practical strategy for promoting the value-added photocatalytic conversion of CO 2 using multivalent transition metal oxide composite photocatalysts. Co 3 O 4 /TiO 2 enables highly selective photoreduction of CO 2 into CH 4 . Ti-O-Co bonds serve as pathways transferring photogenerated electrons from TiO 2 to Co sites. The electron-rich Co centers act as active sites to stabilize *CO intermediates. Meanwhile, Co 3 O 4 promotes water oxidation and maintains sufficient proton supply, synergistically facilitating CH 4 production. Download: Download high-res image (200KB) Download: Download full-size image
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JOURNAL OF MATERIALS SCIENCE
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2026
·
IF 4.4
Li Shiheng,Li Wei,Zhang Baojing,Wang Xiaohong,Feng Peizhong
The widespread application of solid amine adsorbents is hindered by the cost and complexity of synthesizing porous supports, which typically require templating agents and energy-intensive calcination. Herein, we report a facile and mild method to fabricate nanoporous silica, involving CO 2 -induced gelation of low-cost sodium metasilicate, followed by freeze-drying. The obtained silica support exhibits a pore volume of 1.22 cm 3 /g and a specific surface area of 378.5 m 2 /g, which is suitable for amine loading. After impregnation with tetraethylenepentamine, the optimal adsorbent with 50% tetraethylenepentamine loading delivers a competitive CO 2 adsorption capacity of 3.48 mmol/g at 70 °C. More importantly, it demonstrates exceptional cycling stability, maintaining 3.37 mmol/g of CO 2 adsorption capacity after 10 cycles, with a minimal capacity loss of only 0.3% per cycle. This work demonstrates that high-performance adsorbents can be fabricated via a drastically simplified process, offering an amenable to scale-up and economically attractive strategy for practical CO 2 capture. Graphical abstract This paper presents an innovative and template-free synthesis of a high-performance solid amine adsorbent for CO 2 capture. The method innovatively utilizes CO 2 as both a reactant and an in-situ porogen to fabricate nanoporous silica from sodium silicate via a simple one-pot gelation process, entirely bypassing the need for templating agents and energy-intensive calcination. After freeze-drying and tetraethylenepentamine (TEPA) impregnation, the optimal adsorbent with 50% TEPA loading achieves a high CO 2 capacity of 3.48 mmol/g at 70 °C and demonstrates exceptional cyclic stability with 96.8% capacity retention after 10 cycles. This study provides a simplified, cost-effective, and scalable pathway for practical carbon capture applications.
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Science China-Chemistry
·
2026
·
IF 9.8
Wang Nan,An Tinghui,Li Jiaqi,Wang Yuhao,Xiang Dong,Cai Kedi
Cu-based electrocatalysts are promising for the electrocatalytic CO 2 reduction reaction (eCO 2 RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO 2 pulsed laser (L 4 -Mg/Cu x O) was synthesized for highly selective eCO 2 RR to ethanol (C 2 H 5 OH). The synergistic effect of Mg-doping and transient CO 2 pulsed laser irradiation enables excellent eCO 2 RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C 2 H 5 OH and C 2 products under a high current density of 298.9 mA cm −2 , respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H 2 O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO 2 RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C 2 H 5 OH pathway, thus decoupling the selectivity between C 2 H 5 OH and ethylene. When employed in Li-CO 2 batteries, L 4 -Mg/Cu x O delivers 20480 mAh g −1 discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO 2 RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Ye Qu,Yanglin Chen,Yifei Ye,Ping Xu,Jianmin Sun
Heterogenization of homogeneous catalysts without the loss of activity is still a huge challenge. Herein, homogeneous [HTMG][His][I] amino acid ionic liquid (IL), consisting of 1,1,3,3-tetramethylguanidine cation, histidine anion and iodine anion, were introduced into the pore channels of SBA-15 substrate with the assistance of supercritical CO 2 (scCO 2 ) media. Due to its low viscosity, high diffusivity and absence of surface tension, scCO 2 enabled [HTMG][His][I] to highly disperse in SBA-15 pore channels. Surprisingly, [HTMG][His][I]/SBA-15 heterogeneous catalyst displayed higher CO 2 cycloaddition activity (95% propylene carbonate yield) than equivalent molar pristine [HTMG][His][I] homogeneous catalyst (69% propylene carbonate yield) under the identical conditions. The significantly enhanced activity was resulted from the synergistic effect of [HTMG][His][I] and SBA-15 support. Moreover, [HTMG][His][I]/SBA-15 performed outstanding universality of various epoxides and reusability. This work developed a promising strategy to heterogenization of homogeneous IL catalyst assisted by scCO 2 as synthetic media and provided an efficient catalyst for CO 2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Yichen Jiang,Dazhi Li,Yifei Zhao,Jianmin Sun
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2 ). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin , 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br - , together with the high surface area (1178 m 2 /g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yongbiao Sun,Hui Li,Haijun Lai,Yan Yu,Meiling Hou,Chao Fu,Zaizhou Wang,Chunxiang Zhang
Natural gas purification before liquefaction necessitates the use of efficient adsorbents with high selective CO 2 adsorption and easy regeneration. Because of its efficiency and ease of operation, the ion exchange is widely employed to adjust zeolites’ CO 2 adsorption. However, few in-depth mechanistic studies have been undertaken on cation substitution regulation of pore structure and gas–solid interaction, as well as their synergistic effects on CO 2 selective adsorption and zeolite regeneration. In this study, we synthesized Li + and K + -modified 13X and examined their material characteristics, thermodynamics, adsorption kinetics, and the adsorption–desorption performance under various desorption methods. The results showed that the variation in pore structure and gas–solid interaction with cation radius is non-monotonic, resulting in 13XLi and 13XK having better CO 2 selective adsorption than 13X. All zeolites are extremely stable after 10 adsorption–desorption cycles in each regeneration setting. 13X outperforms 13XLi and 13XK in CO 2 desorption at 30 °C, owing to its large non-micropore volume and low gas–solid interaction. 13XK has the lowest CO 2 desorption rate at low temperature but the highest at high temperature, owing to the flat micropore distribution and the progressive gas–solid interaction. Approximately 100 % regeneration of 13XK is achieved with CH 4 purging (150 mL/min) at 150 °C, owing to its smallest cumulative pore volume at 0.5 nm. This research could help to develop efficient cation-modified X zeolites for CO 2 deep removal from CH 4 streams prior to liquefaction, as well as advance the in-depth understanding of cation substitution mechanisms.
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FUEL
·
2022
·
IF 8.035
Yi-Ming Gu,Ya-Hui Wang,Sheng-Sheng Zhao,Hong-Jun Fan,Xiao-Wei Liu,Zhiping Lai,Shu-Dong Wang
Carbon capture from flue gases is one of the crucial routines for reducing current CO 2 emissions and mitigating the greenhouse effect. Metal-organic frameworks (MOFs) have received a lot of interest as efficient solid adsorbents for CO 2 /N 2 separation in flue gas treatment. However, many MOF materials are susceptible to the presence of water vapor, which has a significant impact on their adsorption efficacy and moisture stability. Here in this work, we reported two pillar-layered Zn-MOFs with N -donors, i.e., Zn 2 (TRZ) 2 (Fuma) and Zn 2 (TRZ) 2 (BDC), which demonstrated high CO 2 uptakes (3.92 and 1.52 mmol/g) and CO 2 /N 2 (132 and 20.5) adsorption selectivities at 298 K and 101 kPa, among the best comprehensive results reported by far. After seven days of exposure to a 100 % RH environment, it was found that, the Zn-N pillar contributes to the robust structure of MOFs . Furthermore, in-depth theoretical calculations indicated the guest-framework interactions, and dynamic sorption tests confirmed high working capacities (2.78 and 1.14 mmol/g), sufficient water stability and remarkable cycling performance of the studied MOFs under humid ambient conditions. We believe this work provides a routine to prepare robust and promising candidates to address the challenge in carbon capture under humid conditions.
研究领域:
材料科学
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环境科学
·
化学工程
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