JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Rong Rong,Yanwei Sun,Taotao Ji,Yi Liu
Zirconium-based MOF (Zr-MOF) membranes have attracted widespread attention due to their highly tailorable pore aperture and adsorption behavior achieved by functional group decoration and ligand/cluster-missing defect regulation as well as extraordinary chemical/thermal stability. Nevertheless, it has remained a great challenge to further improve the separation performance of Zr-MOF membranes due to very limited available zirconium sources and heating modes. In this study, we prepared polycrystalline UiO-66 membranes exhibiting unprecedented CO 2 /N 2 selectivity (31.3). The use of layered ZrS 2 , a representative of transition-metal dichalcogenides (TMDCs), as zirconium source during tertiary solvothermal growth was found to be indispensable for improving the separation performance of UiO-66 membranes. As far as we know, the CO 2 /N 2 selectivity reported in this study was the highest among all pristine polycrystalline MOF membranes measured under ambient conditions. More importantly, our study highlighted the importance of concurrent metal source and fabrication process innovation in performance enhancement of polycrystalline MOF membranes.
研究领域:
材料科学
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化学工程
·
膜技术
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Nanxin Zheng,Jingyi Zhu,Zhaozhong Yang,Zhiqiang Jiang,Liangping Yi,Xiaogang Li,Chenyu Wu,Yufeng Long,Duo Yi,Liangjie Gou
CO2 foam fracturing technology is an advantageous method for extracting unconventional resources. However, foam fracturing faces challenges, such as high costs, difficulty in handling surfactants, and potential environmental risks. To address these issues, this study combines CO2-responsive surfactants with zwitterionic surfactants to construct a reusable CO2-responsive viscoelastic foam fracturing fluid system. The mechanism of foam stabilization is revealed through the examination of interfacial characteristics, bulk properties, and microstructural features. Furthermore, the study systematically investigates the drainage kinetics of the CO2-responsive viscoelastic foam fracturing fluid under high-temperature and high-pressure conditions, uncovering its unique properties under high-pressure environments and the synergistic enhancement effects of OAB+DOAPA-CO2 (olefinic amine betaine + oleyl amide propyl dimethylamine) at high temperatures. Finally, the performance of the fracturing fluid is tested. It was found that adding DOAPA-CO2 into OAB increases the base-fluid viscosity by 491.64% and extends the drainage half-life by 281.65%. This is primarily due to the formation of pseudogemini surfactants between OAB and DOAPA-CO2, enhancing the foaming ability of the foam fracturing fluid. Additionally, the mixed wormlike micelles formed are stronger, and the network structure is denser, significantly improving foam stability. Interestingly, as pressure increases, the foam stability of this system improves, owing mainly to the swelling of the wormlike micelles; such exceptional stability under high pressure is highly beneficial during fracturing operations. Meanwhile, the activation energies (Ea) for the OAB and OAB+DOAPA-CO2 systems are 579.47 and 1009.73 J/mol, respectively, indicating that pseudogemini surfactants enhance foam thermal resistance. Performance evaluations show that the damage rate of this fracturing fluid is only 6.15%, making it reservoir-friendly. Moreover, by controlling the introduction of CO2/N2, the base fluid can switch between high- and low-viscosity modes, facilitating the recovery of the fracturing fluid. This study provides technical support for reducing costs associated with CO2 utilization (CO2 foam fracturing) and mitigating the environmental risks posed by surfactant discharge.
研究领域:
石油工程
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Shan Yao,Jiahui Liu,Jinyi Tan,Kun Zhao,Zhiqing Lin,Lai-Hon Chung,Yang Zhou,Xinwen Ou,Jun He,Bin Han,Zhifeng Yang
Dual-atom catalysts (DACs) provide great potential for boosted photoreduction of diluted CO 2 , while the significance of inert sites in DACs is still overlooked. Herein, by loading extra Zn atoms into conducive metal-organic frameworks (CMOFs), we elaborately construct a well-defined DACs with a NiZn─O 4 configuration to decipher the critical role of inert Zn sites in DACs. Under visible light irradiation in pure CO 2 , the NiZn─O 4 DACs with the optimal Zn/Ni ratio exert a boosted CO generation rate of 20.17 µmol h −1 with a selectivity of 97%, which is significantly higher than that of the pristine Ni─O 4 single atom catalysts (SACs) and most documented systems. Additionally, in diluted CO 2 , the activity difference between them increases, and the CO selectivity of Ni─O 4 SACs drops from 95% to 88%, while it remains nearly constant (94%) in the NiZn─O 4 DAC-based system. Experiments combined with theoretical analysis demonstrate that the inert Zn sites enhance the electronic density of the coupled Ni sites, which accelerates electron transfer, promotes reduction kinetics, and lowers the energy barrier for the generation of * COOH key intermediate. This work highlights the intrinsic role of inert sites, paving new avenues for designing effective DACs for various applications.
研究领域:
催化化学
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材料科学
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环境化学
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光催化
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二氧化碳利用
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Sheng Li,Xin Yu,Liming Liu,Liqin Zhou,Zhaowei Jia,Jianmin Chen,Zhongxing Zhao,Zhenxia Zhao
Synchronous boosting adsorption and desorption efficiency is a great challenge for CO 2 adsorption capture, especially for metal–organic frameworks (MOFs) having high adsorption uptakes. Herein, a novel “self-supporting foam” strategy is proposed to fabricate a thermally conductive MOFs@boron nitride nanosheets (BNNS) composite foam (MOFs@BNNS-PEI) via polyethyleneimine (PEI) cross-linkage. The “rebar” BNNS and the “aggregate” MOFs are packed against each other to form a self-supporting structure, effectively reducing the reliance on polymers to maintain high MOFs loading. Furthermore, this approach enables the successful fabrication of three different types of typical MOFs, including HKUST-1, MIL-100(Fe), and ZIF-8. This unique design maintains a high specific surface area (SSA) of the MOFs foam and generates nitrogen-rich microporosity contributing to CO 2 adsorption. Additionally, PEI serves as a thermal bridge to reduce the interfacial thermal resistance between BNNS and MOFs, accelerating the thermal desorption of CO 2 within the MOFs foam. Benefiting from these advantages, the MOFs@BNNS-PEI exhibits a higher CO 2 adsorption capacity (1.35–1.42 times that of pure MOFs) and a significant increase in the desorption rate for CO 2 (5.0–5.7 times that of pure MOFs). Thus, the thermally conductive MOFs foam can be a viable option for efficient CO 2 capture in practical applications.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Hong Qian,Binxia Yuan,Yuhao Liu,Rui Zhu,Chengxi Zhang,Hexing Li
Photocatalytic CO2 reduction to renewable fuels presents a promising strategy to mitigate greenhouse effects, yet challenges persist in achieving high efficiency due to CO2’s thermodynamic stability and competitive H2O adsorption. Herein, we develop a superhydrophobic photochromic TiO2/Bi2Wo6 (TBW-2O) nanocomposite that synergistically enhances visible-light-driven CO2 reduction. Dynamic charge management via reversible W6+↔W5+ transitions not only suppresses charge recombination but also facilitates electron transfer for CO2 activation, as evidenced by in situ XPS and EPR. The superhydrophobic surface designed with sodium oleate (water contact angle >150°) selectively enriches CO2 at the active sites compared to H2O (ΔGCO2 = −2.88 eV vs ΔGH2O = −1.17 eV). Dual heterojunction effects (Type II + Z-scheme) between TiO2 and Bi2WO6 optimize light absorption and redox potentials. The optimized TBW-2O achieves exceptional CH4 and CO production rates of 48.09 and 37.40 μmol·g–1·h–1, respectively, representing 19.7- and 6.6-fold enhancements over pure TiO2. Notably, it attains an apparent quantum yield (AQY) of 0.35% (CH4) and 0.32% (CO) at 350 nm without sacrificial agents or noble metals. Combined experimental and theoretical analyses reveal that the W6+/W5+ redox cycle and hydrophobic interface collaboratively promote COOH/CHO intermediate formation, steering the reaction pathway toward CH4. This work provides a design blueprint for multifunctional photocatalysts integrating photochromism and surface wettability control.
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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催化
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物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Ming-Dong Xie,Jia-Meng Sun,Zhong-Hua Zhang,Hong-Qing Liang,Zhi-Kang Xu
Electrochemical CO 2 reduction (CO 2 RR) in acidic media circumvents carbonate crossover and salt precipitation inherent to alkaline and neutral systems, but suffers from low selectivity due to the dominance of hydrogen evolution. While alkali cations suppress proton activity, they inevitably lead to catastrophic (bi)carbonate deposition and electrode flooding. Here, we decouple CO 2 RR from alkali cations by constructing a micro-alkaline catalytic environment using a proton-blocking hydrophobic membrane with tethered cations. We designed a series of quaternized copolymers from dimethylaminoethyl methacrylate and lauryl methacrylate (qDMA-n), where the “cation–hydrophobicity balance” was precisely tuned to optimize the balance between Donnan exclusion and water management. Integrated into a zero-gap membrane electrode assembly electrolyzer, the optimized membrane enabled CO 2 RR on Ag catalysts with a CO faradaic efficiency of 96.9 % and a single-pass conversion efficiency of 92.4 % at 200 mA cm⁻ 2 in pure 0.05 M H 2 SO 4 , maintaining stable operation for over 100 h. Finite element simulations, rotating disk electrode tests and in-situ Raman spectra revealed that the balance between cationic and hydrophobic domains plays a key role in forming a stable micro-alkaline interface despite bulk acidity, leading to effective HER suppression. This work provides a practical and generalizable interface design principle for efficient CO 2 electrolysis in strong acids, offering new opportunities for durable, high-efficiency CO 2 electrolyzers without alkali cations.
研究领域:
电化学
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二氧化碳利用
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材料科学
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膜技术
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可持续能源
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 17
·3475
·
IF 4.6
Xiaoqian Xu,Song Yang,Yixiang Wang,Ying Chen,Assa Aravindh Sasikala Devi,Feng Hu
Silver is a promising electrocatalyst for electrochemical CO2reduction reaction owing to its high selectivity and efficiency for CO production. However, it still faces a fundamental trade-off between reaction activity and stability. Here, we developed a three-dimensional coral-like porous silver (CP-Ag) catalyst through seed-assisted nanoparticle attachment synthesis, which creates a unique architecture featuring interconnected pores and stable grain boundaries (GBs) between constituent Ag nanoparticles (Ag NPs). Compared to normal Ag NPs, CP-Ag demonstrates superior catalytic performance, maintaining >90% Faradaic efficiency (FE) for CO across a wide potential range (−0.6 to −1.0 V vs. RHE) while achieving 2-times higher current density. Importantly, CP-Ag demonstrated an impressive long-term stability by sustaining nearly 90% FE for CO approximately 40 h at a current density of −50 mA cm−2in a flow cell. The enhanced catalytic performance arises from three factors: (1) the three-dimensional coral-like morphology increases accessible active sites and promotes charge transfer efficiency; (2) stable GBs between interconnected nanoparticles increase reaction activity; (3) more moderate binding on Ag (100) preferentially promotes *CO intermediate formation. Our findings highlight the importance of simultaneously engineering both morphological and crystallographic features to optimize silver catalysts for CO2conversion.
研究领域:
材料科学
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电化学
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纳米技术
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催化
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环境科学
·
能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wu Xinhao,Guo Yanan,Sun Zengsen,Xie Fenghua,Guan Daqin,Dai Jie,Yu Fengjiao,Hu Zhiwei,Huang Yu-Cheng,Pao Chih-Wen,Chen Jeng-Lung,Zhou Wei,Shao Zongping
Electrochemical CO 2 reduction (ECR) is highly attractive to curb global warming. The knowledge on the evolution of catalysts and identification of active sites during the reaction is important, but still limited. Here, we report an efficient catalyst (Ag-D) with suitable defect concentration operando formed during ECR within several minutes. Utilizing the powerful fast operando X-ray absorption spectroscopy, the evolving electronic and crystal structures are unraveled under ECR condition. The catalyst exhibits a ~100% faradaic efficiency and negligible performance degradation over a 120-hour test at a moderate overpotential of 0.7 V in an H-cell reactor and a current density of ~180 mA cm −2 at −1.0 V vs. reversible hydrogen electrode in a flow-cell reactor. Density functional theory calculations indicate that the adsorption of intermediate COOH could be enhanced and the free energy of the reaction pathways could be optimized by an appropriate defect concentration, rationalizing the experimental observation.
研究领域:
材料科学
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电化学
·
光谱学
·
催化
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Kai Zhu,Zihan Lin,Xinyi Bai,Fangfang Chang,Qing Zhang,Xiaolei Wang,Zhengyu Bai
Electrocatalytic reduction reaction of CO2 (CO2RR) into value-added multicarbon (C2+) products represents a sustainable strategy for mitigating greenhouse gas emissions and enhancing the production of high-value chemicals. Cu-based catalysts are optimal for the CO2RR, facilitating the generation of C2+ products such as ethanol, which have significant industrial applications. However, converting CO2 to C2+ products remains a great challenge, necessitating the simultaneous achievement of high current density, Faradaic efficiency (FE), and operational stability for industrial-scale implementation. Herein, we prepared Cu/Cu2O catalysts with diverse morphologies and the ratio of the Cu+/Cu interface, which was rectified by regulating the interactions between the active interface and the intermediate (*CO). The electrochemical analysis demonstrated that reconstructed Cu/Cu2O nanodendrites with dominant grain boundaries exhibited remarkable performance in generating C2+ products, achieving a Faradaic efficiency (FE) of 71.8%, including 49.7% FE of ethanol and a substantial partial current density of 390.0 mA cm–2 within the flow cell. In situ spectroscopy characterization and theoretical calculations revealed that the increased ethanol selectivity originated from the rectification of the Cu/Cu2O interface by the *CO intermediate, which accelerated H2O dissociation, reduced the free energy for *CO hydrogenation to *COH, and facilitated asymmetric *CO-*COH coupling to preferentially reduce CO2 to ethanol. This study provides profound insights into the C–C coupling pathways and sheds light on the rational design of ethanol-oriented electrocatalysts, contributing to sustainable chemical synthesis and energy utilization.
研究领域:
电催化
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能量转换
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材料科学
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环境化学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Jiaxin Wang,Ying Liu,Baozhong Zhu,Jiuyu Chen,Qing Wang,Yunlan Sun
Amine-modified mesoporous silicon was widely used for CO 2 capture. However, its adsorption capability was significantly affected by temperature and humidity. In this paper, tetraethylenepentamine (TEPA) modified SBA-15 adsorbents were prepared for capturing CO 2 . The effects of the modification method, the concentration of TEPA, the adsorption temperature, and the humidity of atmosphere on CO 2 adsorption capability were studied. Moreover, combined with molecular dynamics (MD) and density functional theory (DFT) computations, the diffusion characteristics and adsorption mechanism were explored. The CO 2 adsorption capability of the adsorbent prepared by the ultrasonic impregnation method was higher than those prepared by the stirring impregnation method, owing to that ultrasonic impregnation could promote the uniformity of TEPA. With the increase of TEPA concentration of SBA-15, the CO 2 adsorption capability increased. SBA-15-2 had the highest CO 2 adsorption capability of 1.17 mmol/g at 30 °C. This was due to the N-containing functional groups, showing good affinity for CO 2 , introduced by TEPA impregnation. When the temperature increased from 30 °C to 70 °C, the CO 2 adsorption capability of all modified SBA-15 adsorbents decreased, since the CO 2 adsorption was an exothermic reaction. SBA-15-2 showed better water vapor resistance than SBA-15-2 (Stir). This was related to the higher dispersity of organic carbon chain introduced by TEPA modification after ultrasonic impregnation. The organic carbon chain of SBA-15-2 increased the water vapor resistance by reducing the hydroxyl group. Finally, from a microscopic aspect, the MD simulation suggested that impregnated TEPA inside SBA-15 may improve CO 2 capture by increasing the thickness of effective adsorption layer. Besides, the DFT simulation showed that TEPA modification increased the adsorption energy of SBA-15 on CO 2 . This serves as a reference for later mesoporous silicon adsorbent research and development on CO 2 capture.
研究领域:
材料科学
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环境科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER SCIENCE SERIES A
·
2018
·Vol. 60
·期 5
·612-617
·
IF 0.729
Wang Jinjing,Wang Huifeng,Li Yan,Tian Li,Chen Shanmin,Liu Qiang,Guo Zhen
A novel copolymer surfactant has been prepared via a free radical copolymerization of CO 2 -switchable monomer N , N -diethylaminoethyl methacrylate and the hydrophilic monomer sodium vinyl-sulfonate and characterized. The results of conductivity, dynamic light scattering and cryogenic transmission electron microscopy study showed the change of the microstructure of copolymer in water by adding or removing of CO 2 . The copolymer aqueous solution was found to exhibit reversible switchability by the bubbling of CO 2 /N 2 .
研究领域:
高分子化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Wenhao Liu,Qingcai Chen,Tengfei Xu,Sitong Liu,Yifan Sun,Huadong Huang
Low-cost support materials and simple synthesis methods can significantly reduce the cost of solid amine technology, which is crucial for its commercialization. This research work utilized blast furnace slag as raw material and adopted a green, simple treatment method to prepare the support materials (BFSC), which exhibited high specific surface area (238.83 m 2 /g) and pore volume (1.09 cm 3 /g). The main component of the support material is magnesium aluminum metasilicate. The support material was modified with different contents of polyethyleneimine (PEI) and tetraethylenepentamine (TEPA), the results showed that BFSC-50 %TEPA exhibited the best CO 2 adsorption performance (3.27 mmol/g). Subsequently, the effects of adsorption conditions on BFSC-50 %TEPA were investigated, including temperature, humidity, and different gas compositions. In atmosphere condition of 15 % CO 2 and 85 % air (with 60 % humidity), high temperatures promote the formation of a urea derivative, which significantly impairs the material’s CO 2 adsorption capacity. Finally, the cyclic stability of BFSC-50 %TEPA was tested.
研究领域:
环境科学
·
化学工程
·
材料科学
·
碳捕集与封存
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）