CARBOHYDRATE POLYMERS
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2016
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IF 4.219
Jisheng Yang,Hongbiao Dong
A new kind of hexyl diethyl tertiary amine-grafted amphiphilic alginate derivative (HDEA-Alg) was synthesized from (6-bromo-hexyl)-diethyl-amine (BHDEA) and sodium alginate (NaAlg) through esterification. The structure of HDEA-Alg was confirmed by FT-IR and NMR spectroscopies. The grafting ratio was calculated according elemental analysis and thermodynamic property was analyzed by TG. The CO 2 /N 2 -responsive performance of HDEA-Alg in aqueous solution was demonstrated by surface tension and conductivity measurements. Stable emulsions of liquid paraffin were easily prepared in the presence of the HDEA-Alg. These emulsions can be de-emulsified by bubbling CO 2 through the emulsions at 5 °C for 30 min, resulting in complete oil/water phase separations. They can be re-emulsified by bubbling N 2 through the solutions at 50 °C for 30 min with the aid of homogenization.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Peng Zhang,Linglong Wang,Jiansong Miao,Tao Gan,Bangyan Zhang,Guanna Li,Chunming Xu,Xiaohui Sun
Dual-atom catalysts (DACs) with unique interactions between neighboring sites are promising candidates in the electrocatalytic CO 2 reduction reaction (CO 2 RR). Yet, the controlled synthesis of pure DACs remains a challenge to date. Herein, we propose a facile cation–anion pair adsorption-pyrolysis approach to fabricate a nitrogen-doped carbon supported Fe DAC. Based on this strategy, Fe 2 pairs can be homogeneously incorporated into the carbon substrate. When this candidate was evaluated in the electrocatalytic CO 2 RR, it exhibited a CO faradaic efficiency ( FE CO ) of ∼97 % at an industrial current density of 200 mA cm −2 in a gas diffusion electrode (GDE)-based flow cell filled with 0.5 M KHCO 3 electrolyte, surpassing most of the reported Fe based SACs. Experiments combined with theory revealed that the Fe 2 pair with enhanced electronic localization lowered the reaction free energy for COOH* formation on Fe, thereby boosting the catalytic performance in CO 2 RR. The structure–property relationship built in this study offers atomic-level insights into the rational design of electrocatalysts for efficient CO 2 RR, and extends the application of DACs for heterogeneous electrocatalysis and beyond.
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iScience
·
2025
·
IF 4.1
Kai Chen,Jia−Yi Du,Haoran Zhang,Yingqi Fan,Dong−Yue Yang,Jin Wang,Kai Li,Gang Huang
Lithium (Li)−CO 2 batteries, capable of converting CO 2 to Li 2 CO 3 /C while delivering significant energy, have attracted extensive research interest. However, their feasibility remains controversial and underexplored. To address this, a rigorous testing system combining ECC−Air battery models and differential electrochemical mass spectrometry (DEMS) was developed to ensure a pure gas environment. Findings reveal that even minute O 2 permeation (0.5%) from air can elevate the discharge plateau, misleadingly transforming Li−CO 2 into Li−O 2 /CO 2 batteries. Under strict testing, true Li−CO 2 battery performance falls short of reported successes. Experimental and theoretical confirmation shows the 4Li + 3CO 2 → 2Li 2 CO 3 + C reaction proceeds at a lower discharge plateau (<2.0 V), a voltage window traditionally overlooked. This work underscores the need for rigorous testing to enhance scientific reliability in Li−CO 2 battery research so that this field can develop sustainably.
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PubMed
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Sustainable Energy & Fuels
·
2025
·
IF 4.1
Yongheng Xiong,Yang Yu,Huangang Shi,Jifa Qu,Wenyi Tan
Single atom Fe sites, doped in CN materials, exhibit outstanding electrochemical activity for CO2-to-CO conversion. The pyrolysis of ZIF8 is a controllable method for fabricating isolated single atom metal sites. In this study, we propose a new strategy to increase the ratio of Fe in ZIF8 precursors by synergistically replacing Zn2+ with Bi3+ and Fe3+. After precursor pyrolysis, the obtained Bi/Fe–N–C catalysts, consisting of Bi sites and pyrrole-type Fe–Nx sites, serve as efficient electrocatalysts for the CO2RR. The results show that the optimized catalyst loaded with 94.8 mg per kgCat Fe exhibits a high FECO of >90.1% over a wide potential range of −0.4 to −0.7 VRHE (98.2% at −0.5 VRHE). Insights into the electrochemical reaction mechanism show that this successful design of Bi/Fe–N–C catalysts can provide a stable catalytic site to form *COOH, thus achieving energy-efficient electrochemical CO2 reduction to CO.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Meisi Chen,Tong Zhao,Zekai Jin,Bing Yu,Ren Xiong,Muhua Chen,Xinbao Zhu,Bo Fu
s To develop high-performance and green CO 2 adsorbent materials, this study introduces a dual-amine synergy strategy. A composite material was constructed by in-situ growth of NH 2 -MIL-53 on a polyethyleneimine (PEI)-functionalized porous cellulose paper, achieving a mechanically robust adsorbent with a hierarchical pore structure. Benefiting from the synergistic effect between MOF and PEI amine sites, the composite paper PNMP-3 exhibited a CO 2 adsorption capacity of 1.71 mmol/g (52 % higher than the unmodified sample), a CO 2 /N 2 selectivity of 138.4 and excellent cyclic stability. Furthermore, theoretical simulation calculations revealed that the high capacity stems from hydrogen bonding between dual amino sites and CO 2 , while the high selectivity is due to the enhanced CO 2 binding energy. This design, integrating synergistic adsorption sites with hierarchical pores, offers an efficient pathway for green carbon capture materials.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kejin Yan,Haoyu Jiang,Shuai Yin,Yunhao Zhang,Yiheng Gong,Haijun Chen,Hao Peng
This study develops a novel microencapsulated carbon sorbent (MECS) by integrating a composite Na 2 CO 3 -MEA (monoethanolamine) absorbent with droplet microfluidics technology. Building upon the activation mechanism of MEA, the CO 2 absorption performances of Na 2 CO 3 -MEA composites at different molar ratios are systematically investigated. A multi-objective optimization function identifies an optimal composition that achieves a 149 % increase in CO 2 capture rate compared to Na 2 CO 3 solution alone, while maintaining excellent cost-effectiveness. Subsequently, this high-performance absorbent is encapsulated within a photocurable organosilicone shell via a triple-coaxial capillary microfluidic device, forming stable core-shell microcapsules (MECS@Na 2 CO 3 –MEA). By leveraging hydrodynamic tuning, we achieved precise control over the microcapsule's geometry, systematically tuning shell thickness and particle size to fundamentally optimize the performance for CO 2 absorption. Under a pressure of 0.7 atm and an optimized temperature of 40 °C, the MECS@Na 2 CO 3 –MEA demonstrates a 36 % higher CO 2 absorption capacity compared to an equivalent mass of the unencapsulated absorbent. This significant enhancement persists even under low CO 2 concentration conditions, where 33 % and 57 % improvement are observed at 1 vol% and 5 vol% CO 2 , respectively. Furthermore, the microfluidic fabrication method also permits the incorporation of magnetic nanoparticles, endowing the MECS with dual functionality: magnetic responsiveness that enables remote steering and further improves CO 2 absorption performance. This work presents a promising, cost-effective approach for developing high-performance materials for carbon capture applications.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Dingming Xue,Xiaofei Yan,Fei Liu,Mengqi Liu,Houhu Zhang
The photocatalytic performance of covalent organic frameworks (COFs) is fundamentally constrained by high exciton binding energies (Eb), which impede efficient exciton dissociation and kinetically retard free-charge carrier generation. In this study, we report the first successful integration of an anthrathiophene unit into a COF backbone, constructing a COF (TA-COF) with an extended π-conjugated system. Concurrently, we developed two distinct COF variants, TF-COF (pyrene-core) and TP-COF (benzene-core), with systematically modulated π-conjugation intensities to enable comparative analysis. The research results indicate that TA-COF, featuring an anthrathiophene-based core, achieved the expanded light response, lower Eb, and accelerated charge transfer impetus and reduced energy barrier of the rate-determining step, finally enabling efficient exciton dissociation, charge separation, and the improvement of photocatalytic activity. TA-COF exhibited exceptional photocatalytic CO2-to-CO reduction activity (301.5 μmol·g–1·h–1) with >90% selectivity under visible light. This work establishes conjugation engineering as a critical lever for optimizing exciton dynamics in COF-based photocatalysis.
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AICHE JOURNAL
·
2025
·
IF 4
Mengjiao Zhang,Tianbao Shi,Yitong Li,Bin Liu,Zhiwu Liang,Paitoon Tontiwachwuthikul,Jin-Heng Li
Amine-based chemical absorption remains a promisingly powerful technology for carbon dioxide (CO 2 ) capture. However, enhancing the performance of absorbents remains a significant challenge. In this study, three sterically hindered amines (SHAs), including 2-( tert -butylamino)ethanol, 2-amino-2-methyl-1-propanol, 2-amino-2-methylpropane-1,3-diol were selected as the primary absorbents with piperazine (PZ) employed as an activator. Absorption and desorption experiments were conducted for various PZ-SHAs systems with a total amine concentration of 30 wt% under conditions of 313 K and 13 kPa CO 2 partial pressure. The CO 2 absorption capacity, initial absorption rate, desorption rate, and desorption energy consumption were systematically evaluated, indicating that the addition of PZ as an activator could effectively improve the trapping capacity of the spatially hindered amine, and keep a high recycling capacity and low regeneration energy. Finally, the CO 2 reaction mechanism under the new system was clarified by 13 C nuclear magnetic resonance (NMR) technique.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Yuqing Wang,Shaojun Jia,Wu Chen,Yi Li,Yao Jiang,Peng Cui
CO 2 phase change absorbents (CPCA) have attracted significant interest as potential candidates for the high-efficiency capture of CO 2 . However, the high viscosity of the rich phase in CPCAs hinders their broader application. Given the exceptional CO 2 capture performance and cyclic stability of piperazine (PZ), this study focuses on developing a PZ-based CPCA system of PZ/ n -BuOH/H 2 O to reduce solution viscosity and regeneration energy consumption. Experimental results reveal that the viscosity of the rich phase in PZ/ n -BuOH/H 2 O is as low as 7.06 mPa·s, while the regeneration energy consumption is 2.64 GJ·t −1 CO 2 , which is 19.8 % lower than in the conventional PZ/H 2 O system. Furthermore, 13 C NMR analysis and density functional theory (DFT) calculations provide insight into the CO 2 capture process and mechanism of PZ/ n -BuOH/H 2 O, indicating that polarity differences are primarily responsible for phase separation. Overall, the CPCA of PZ/ n -BuOH/H 2 O developed in this study evinces considerable potential for industrial CO 2 capture applications.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Yongxian Liu,Zhihua Feng,Zhangting Dang,Qingqing Hou,Yue Yu,Xiaofei Zhao,Lingling Wang,Yong He,Renbo Wei,Xiufu Hua
Converting CO 2 efficiently into high-value-added chemical products represents dual value in ecological conservation and resource valorization. Designing novel catalysts integrating atom economy and process intensification constitutes the cornerstone for catalytic CO 2 conversion. Herein, an integrated polymeric heterogeneous catalyst is constructed by covalently anchoring functional groups of quaternary ammonium (QA) and copper phthalocyanine (CuPc) onto a polyurea (PU) framework, yielding PU-CuPc-QA. This catalyst is subsequently applied for CO 2 conversion to cyclic carbonates. Owing to the Cu 2+ centers in phthalocyanine and urea groups from PU acting as a Lewis acid and hydrogen bond donor (HBD) to efficiently activate epoxide, as well as nucleophilic attack of this activated epoxide by iodide ion (I - ) dissociated from QA, PU-CuPc-QA facilitates ring-opening of epoxide. Moreover, the phthalocyanine rins and the QA cations in PU-CuPc-QA work as N -rich groups that can adsorb and active CO 2 . As a result, PU-CuPc-QA exhibits exceptional catalytic activity for CO 2 cycloaddition under mild conditions without adding any external co-catalysts. Specially, at 100 o C, 1.5 MPa of CO 2 , 6%(mass) PU-CuPc-QA achieve 99% propylene carbonate yield and selectivity after reacting with propylene oxide for 6 h. Combining its ability to catalyze and activate epoxide and CO 2 simultaneously, PU-CuPc-QA is a promising catalyst for CO 2 cycloaddition.
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Catalysts
·
2025
·Vol. 15
·期 11
·1037
·
IF 4
Ming Cai,Shaokun Lv,Yuanyuan Li,Wahyu Prasetyo Utomo,Yongsheng Yan,Zhi Zhu,Jun Zhao
Photocatalytic CO2reduction holds great potential for sustainable solar fuel production, yet its practical application is often limited by inefficient charge separation and poor product selectivity. The photothermal effect presents a viable strategy to address these challenges by reducing activation energies and accelerating reaction kinetics. In this work, we report a rationally designed CN-B/Ti3C2heterojunction that effectively leverages photothermal promotion for enhanced CO2reduction. The black carbon nitride (CN-B) framework, synthesized via a one-step calcination of urea and Phloxine B, exhibits outstanding photothermal conversion, reaching 131.4 °C under 300 mW cm−2illumination, which facilitates CO2adsorption and charge separation. Coupled with Ti3C2MXene, the optimized composite (3:1) achieves remarkable CO and CH4production rates of 80.21 and 35.13 μmol g−1h−1, respectively, without any cocatalyst—representing a 2.9-fold and 8.8-fold enhancement over CN-B and g-C3N4in CO yield. Mechanistic studies reveal that the improved performance stems from synergistic effects: a built-in electric field prolongs charge carrier lifetime (3.15 ns) and reduces interfacial resistance, while localized heating under full-spectrum light further promotes CO2activation. In situ Fourier transform infrared (FTIR) spectroscopy confirms the accelerated formation of key intermediates (*COOH and *CO). The catalyst also maintains excellent stability over 24 h. This study demonstrates the promise of combining photothermal effects with heterojunction engineering for efficient and durable CO2photoreduction.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Kaiyu Ma,Jing Wang,Yue Ju,Lei Chen,Xinyu Song,Weiwen Zhang
With the increasing restrictions on petrochemical-derived polymers and growing demand for sustainable materials, cis, cis-muconate (ccMA) has emerged in recent years as a promising platform chemical for green manufacturing. However, ccMA biosynthesis in heterotrophic microorganisms still consumes sugar- or lignin-derived feedstocks, which constrains its sustainability profile and prevents it from being a truly green or carbon-negative process. Although photosynthetic microorganisms can be engineered as “negative-carbon factories” to convert photosynthetically fixed CO2 into diverse value-added products, the direct synthesis of ccMA has so far been precluded by intrinsic metabolic limitations, including the feedback-regulated and largely unexplored shikimate pathway as well as an NADPH/ATP imbalance that conflicts with high NADPH demand of ccMA biosynthesis. This study presents a two-species, three-module design for sustainable ccMA biomanufacturing. Specifically, a model photosynthetic chassis Synechococcus elongatus PCC 7942 was engineered with sucrose and trans-cinnamic acid module to supply carbon and engery, while the heterophic chassis Corynebacterium glutamicum ATCC 13032 carried a reonstructed shikimate module for ccMA synthesis. This modular distribution not only alleviated metabolic burden in individual strains but also enhanced system robustness through rational medium optimization, fine-tuned inoculation ratios, and spatial stabilization of cyanobacteria using sodium alginate hydrogel immobilization. While the titers remain modest (7.04 and 8.61 mg L⁻1 under non-immobilization and immobilization, respectively), this proof-of-concept system achieved a net carbon reduction of −15.10 kg CO2e kg-1 of produced ccMA, highlighting its environmental advantages and potential for carbon-negative biomanufacturing.
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