FUEL
·
2025
·
IF 7.5
Xiaochao Xu,Jiaxin Zou,Zhen Xiao,Jiangjie zhang,Bing Wang,Jianing Jiang,Jinni Shen,Lifang Yang,Wenxin Dai,Zizhong Zhang
Controlling the crystallinity and microstructure of a semiconductor photocatalyst serves as an effective means to boost its photocatalytic performance through improving the charge transfer and separation, enhancing the light absorption, or maneuvering the surface reactions. Nevertheless, the internal pores in aerogel materials inevitably collapse during the traditional high temperature crystallization process, significantly reducing the porous structure and specific surface area (SSA). Herein, microsphere ZnO aerogels have been successfully fabricated for photoreduction of CO 2 using a cooperative strategy of sol–gel method, solvothermal crystallization and cryodesiccation. The obtained aerogel has a large SSA and high crystallinity. Compared with the commercial ZnO powder, the ZnO aerogel microsphere exhibits about 4-fold increase in specific surface area, leading to an increased contact surface between the photocatalyst and the reactant. At the same time, ZnO aerogel with microsphere morphology possesses high light-harvesting and intrapore light reflecting capabilities, demonstrating enhanced optical utilization. Modulation of the crystallinity of ZnO aerogel facilitated the incorporation of defect engineering (zinc defects (Zn i ) and oxygen vacancies (V o )). As a result, ZnO aerogel microsphere exhibits a 5-fold higher products production rate than ZnO powder for photocatalytic CO 2 reactions due to the synergistic effect of appropriate crystallinity and microsphere appearance. It is hoped that this work may provide some insights to tune the catalyst performance through crystallinity and morphology.
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高影响因子
Natural Gas Industry B
·
2025
·
IF 6.5
Mingwei Zhao,Yizheng Zhang,Xiangjuan Meng,Xuguang Song,Yingnan Wang,Zixuan Wang,Caili Dai
CO 2 foam fracturing fluid can effectively integrate CCUS technology into oil and gas field development, and its core advantages include low water consumption, excellent flowback performance, and strong sand-carrying capacity. For these reasons, it has received increasing attention in the oil and gas field development field. However, this type of fracturing fluid still has some prominent problems: The residue from gel breaking can easily cause formation pollution, the system cost is relatively high, and the utilization rate is low, which forms a significant technical bottleneck. In response to these issues, this study, based on the theory of clean fracturing fluid gel breaking without residue and the reusability of CO 2 -responsive wormlike micelles, innovatively combines CO 2 -responsive wormlike micelles with different types of surfactant-based foaming agents to construct a new CO 2 -responsive foam fracturing fluid system. A systematic performance evaluation of the system was conducted to clarify its defoaming rules under different temperature conditions. Compared with the traditional guar gum CO 2 foam fracturing fluid, the new system has significant performance advantages. At 90 °C, its foam comprehensive value reached 19720 mL·min, 6150 mL·min higher than the guar gum fluid. After a 5400 s high-temperature and high-shear test at the same temperature, the residual viscosity of the new system was 67 mPa·s, which is higher than the guar gum fluid. This CO 2 -responsive foam fracturing fluid simultaneously possesses the application potential of both clean fracturing fluid and foam fracturing fluid. It can effectively solve key problems such as formation pollution and low system utilization rates, and laboratory evaluation experiments confirmed its excellent foaming and rheological properties. These results are of great significance for promoting CO 2 foam fracturing technology to reach an advanced international level and supporting the low-carbon and high-efficiency development of unconventional oil and gas resources in China.
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高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 46
·e04276
·
IF 2
Changle Wang,Zhijing Liang,Cuizhen Bai,Jiong Sun,Salman Qadir,Yuhe Liao,Congguang Zhang,Muhammad Sajjad,Haiming Yang,Shao-Tao Bai
Typically, SiO 2 , Al 2 O 3 , MOF, and polymers are used to prepare solid amine CO 2 adsorbents. In this manuscript, we explored abundant lignin waste to prepare a series of solid amine CO 2 adsorbents via in situ Mannich reactions with commercially available, cheap ethanolamine and polyethyleneimine. Upon optimization of amine loadings and reaction conditions, the novel ethanolamine modified adsorbents showed significantly improved CO 2 capture performance (6.83 mmol/g) compared to native lignin (2.57 mmol/g) under laboratory testing conditions (25 ° C, 1 bar, and 10 vol% CO 2 /Ar). Unfortunately, the captured CO 2 can be regenerated with a maximum limit of 50% under rather harsh conditions, implying likely utilization of the cheap adsorbents loaded with CO 2 as building fillers and adhesives. Elemental analysis, scanning electron microscopy, x-ray photoelectron spectroscopy, thermogravimetric analyzer, CO 2 adsorption isotherm, and Fourier transform infrared spectrometer analysis were applied to characterize the texture properties and CO 2 capture mechanisms.
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高影响因子
ACS Nano
·
2025
·
IF 16
Chengbo Li,Xian Zhong,Yuan Ji,Yawei Hong,Jiawei Li,Youpeng Wang,Hongliang Zeng,Chunxiao Liu,Zhaoyang Chen,Xu Li,Qiu Jiang,Tingting Zheng,Hong-Jie Peng,Xinyan Liu,Chuan Xia
The electrochemical conversion of CO2 into valuable chemicals under acidic conditions provides a promising solution to challenges, such as carbon loss and catalyst instability caused by carbonate precipitation. However, acidic CO2 electroreduction remains severely constrained by intense competition from the hydrogen evolution reaction (HER) and sluggish CO2 activation kinetics. Here, we report a bismuth (Bi) nanoparticle catalyst with an amorphous surface layer (a-Bi), which demonstrates high catalytic activity and selectivity toward formic acid (HCOOH) formation in acidic electrolytes. The catalyst achieves impressive Faradaic efficiencies for HCOOH production, exceeding 90% over a wide current density range (−100 to −1000 mA cm–2) with corresponding potentials ranging from −1.24 to −1.75 V versus the reversible hydrogen electrode (vs RHE). Notably, the partial current density for an HCOOH reaches an impressive value of more than −900 mA cm–2 at −1.75 V vs RHE. Furthermore, the a-Bi catalyst exhibited stability for over 52 h at high production rates (−500 mA cm–2) alongside a single-pass carbon efficiency of approximately 85%. In situ spectroscopy and theoretical simulation revealed that surface amorphization significantly enhances the adsorption of CO2 and lowers the hydrogenation barrier, thereby accelerating the CO2RR kinetics while effectively suppressing the HER. This work presents a facile crystallization engineering strategy to address critical carbon loss challenges, thereby advancing the sustainability and scalability of acidic CO2 electroreduction processes.
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Xiangyue Ye,Jiemei Zhou,Chenxu Zhang,Yong Wang
The intelligent responsive membranes have aroused much attention due to their distinctive capability to reversibly change separation performances under the stimulation of ambient environment. Especially, the responsive membranes derived from block copolymers , which have regular nanoporous structures, display great potential in high-precision controllable separation. Herein, we use CO 2 gas as the non-toxic, mild stimulus, and develop the responsive membranes from a block copolymer of poly(2-diethylaminoethyl methacrylate)-block-polystyrene (PDEAEMA- b -PS) by the selective swelling method. The membranes exhibit a bi-continuous nanoporous structure and the surfaces and pore walls are rich with CO 2 -responsive PDEAEMA chains. Based on the reversible conformation transition of PDEAEMA chains between the collapsed state and extended state upon CO 2 /N 2 stimulation, the membranes achieve the controllable regulation on the water permeances from ∼100 to ∼2100 L⋅h −1 ⋅m −2 ⋅bar −1 , also realize the blocking/passing switch for varied proteins. More importantly, the extended PDEAEMA chains shrink the effective pore size down to less than 5 nm, moving the separation scope from ultrafiltration to tight-ultrafiltration. Thus, the membranes are capable to separate macromolecular proteins with small molecule polypeptide and vitamin with high separation efficiencies, demonstrating their application prospect in precise separation and fractionation of biomolecules.
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高影响因子
JOURNAL OF PHYSICAL CHEMISTRY B
·
2019
·
IF 2.923
Ying Zhang,Dongfang Liu,Shanshan Dai,Hongsheng Lu
A novel surfactant-free microemulsion (SFME) based on CO2-induced ionic liquids (ILs) was prepared. Among them, dipropylamine (DPA) was directly reacted with CO2 to form the ILs that were composed of the ammonium salts and the ammonium carbamate salts, which was confirmed by 13C NMR, Fourier transform infrared, electrical conductivity, and pH. In addition, the purity of ILs was determined by 1H NMR. We used water as a polar phase, ILs as an amphi-solvent, and 1-dodecanol as a nonpolar phase to prepare SFME. The multiphase zone and the single-phase zone of the SFME were obtained from the ternary-phase diagram. Then, the microstructure of the studied SFME was determined to be the O/W type by the staining method. The demulsification process of SFME was explored by means of conductivity, pH, dynamic light scattering, and gas chromatography. Under the introduction of N2, CO2 could be removed, and the ILs could be reversibly restored to DPA, resulting in a change in polarity, which caused most of DPA to transfer into the oil phase, eventually leading to demulsification.
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DOI
PubMed
高影响因子
Fundamental Research
·
2021
·
IF 0
Wanyu Deng,Tenghui Yuan,Sai Chen,Huimin Li,Congling Hu,Hao Dong,Bo Wu,Tuo Wang,Jingkun Li,Geoffrey A. Ozin,Jinlong Gong
CO 2 electroreduction (CO 2 ER) using renewable energy is ideal for mitigating the greenhouse effect and closing the carbon cycle. Bicarbonate (HCO 3 − ) is most commonly employed as the electrolyte anion because it is known to facilitate CO 2 ER. However, its dynamics in the electric double layer remains obscure and requires more in-depth investigation. Herein, we investigate the refined reduction process of bicarbonate by employing in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy. By comparing the product distributions in Ar-saturated KCl and KHCO 3 electrolytes, we confirmed CO production from HCO 3 − in the absence of an external CO 2 source. Notably, in contrast to an electric compulsion, negatively charged HCO 3 − anions were found to accumulate near the electrode surface. A reduction mechanism of HCO 3 − is proposed in that HCO 3 − is not adsorbed over a catalyst, but may be enriched near the electrode surface and converted to CO 2 and react over Au and Cu electrodes. The dependence of the CO 2 ER activity on the local HCO 3 − concentration was subsequently discovered, which was in turn dependent on the bulk HCO 3 − concentration and cathodic potential. In particular, the local HCO 3 − concentration was limited by the cathodic potential, leading to a plateau in the CO 2 ER activity. The proposed mechanism provides insights into the interaction between the catalyst and the electrolyte in CO 2 ER.
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DOI
Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Meng Zhao,Dong-Dong Zhou,Pin Chen,Yujie Ban,Yuecheng Wang,Ziyi Hu,Yutong Lu,Mu-Yang Zhou,Xiao-Ming Chen,Weishen Yang
Hydrogen/carbon dioxide (H 2 /CO 2 ) separation for sustainable energy is in desperate need of reliable membranes at high temperatures. Molecular sieve membranes take their nanopores to differentiate sizes between H 2 and CO 2 but have compromised at a marked loss of selectivity at high temperatures owing to diffusion activation of CO 2 . We used molecule gatekeepers that were locked in the cavities of the metal-organic framework membrane to meet this challenge. Ab initio calculations and in situ characterizations demonstrate that the molecule gatekeepers make a notable move at high temperatures to dynamically reshape the sieving apertures as being extremely tight for CO 2 and restitute with cool conditions. The H 2 /CO 2 selectivity was improved by an order of magnitude at 513 kelvin (K) relative to that at the ambient temperature.
研究领域:
膜科学
·
材料科学
·
能源可持续性
·
气体分离
·
计算化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Liang Cai,Guangfan Tan,Xiuhong Yang,Haifeng Xue,Yitong Lin,Xin Hu,Zhuoyuan Song,Yingchun Zhang
Li 4 SiO 4 is considered as one of the most promising materials for post-combustion CO 2 capture at high temperature due to its inherent merits. To avoid elutriation in practical application, granulating and shaping of Li 4 SiO 4 sorbents are getting extensive attention. However, the cylindrical or spherical pellets prepared by traditional methods are prone to result in severe damping of CO 2 capture performance. In this work, the cellular structure Li 4 SiO 4 sorbent was firstly yielded by additive manufacturing based on polymer-derived ceramics strategy. The phase evolution and calcination process were investigated to optimize the microstructure of that sorbents. In addition, three sodium halides were severally doping in Li 4 SiO 4 sorbents to further improve the CO 2 uptake, and the enhancement mechanism was studied. Results show that abundant gas channels around the Li 4 SiO 4 grain can be generated by a novel residual carbon controlling calcination. Additionally, the 6 mol% NaF doped cellular structure Li 4 SiO 4 sorbents possessed superior CO 2 adsorption capacity: 0.329 g CO2 /g sorbent in 70 vol% CO 2 and 0.286 g CO2 /g sorbent in 15 vol% CO 2 , as well as ultrafast adsorption rate. Especially, the sorbents still kept a high adsorption capacity of 0.274 g CO2 /g sorbent and obtained a more efficient regeneration process after undergoing 15 cycles of adsorption–desorption in a low CO 2 concentration flue gas. Hence, the introduction of additive manufacturing and polymer-derived ceramics strategy in fabrication of Li 4 SiO 4 sorbents provides a new approach and promising prospects for the high-temperature CO 2 capture.
研究领域:
材料科学
·
环境工程
·
化学工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hang Shi,Cheng Tian,Xianglei Liu,Nan Sun,Chao Song,Hangbin Zheng,Ke Gao,Xinrui Wang,Zhixing Jiang,Yimin Xuan,Yulong Ding
Solar-driven CO 2 reduction by methane (CRM) into valuable syngas not only mitigates greenhouse gases but also provides high-value syngas. However, it is still a daunting challenge to achieve high solar-to-fuel efficiency and good durability simultaneously. Here, a novel strategy of direct photothermocatalytic CO 2 is proposed based on a unique nanocomposite of ceria coated Ni-phyllosilicate nanotubes (Ni-psnts@CeO 2 ). A record-high solar-to-fuel efficiency (36.9 %) with very high production rates of H 2 and CO (120.90 and 136.84 mmol g cat min −1 ) and high CO 2 conversion rate (90.4 %) close to thermodynamic limit are demonstrated. Excellent long-term durability is achieved due to its extremely low carbon deposition rate of 1.3 × 10 −4 g c g cat h −1 under focused UV–vis-IR irradiation for 100 h. These high performances are partially attributed to the active involving of lattice oxygen and oxygen vacancies from ceria in carbon gasification and CO 2 activation, which are confirmed by 18 O isotope labeling and In-situ DRIFTS measurements. In addition, decreased activation energy enabled via photoactivation effects from photoexcited hot electrons also benefits high activities under direct light illumination. This work offers novel approaches for highly efficient and stable solar-driven CO 2 -to-fuel conversion.
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高影响因子
CRYSTENGCOMM
·
2023
·Vol. 26
·期 1
·70-79
·
IF 3.1
Zhen Li,Bo He,Shaokun Tang
Hierarchically porous metal–organic frameworks (HP-MOFs) possess the advantages of the high porosity of MOFs and unique properties, such as a wide pore size range. Hierarchically porous ZIF-8 (HP-ZIF-8) was facilely fabricated via a one-step method in supercritical CO2 (scCO2) using a competitive ligand. The mesoporous structure and morphology of HP-ZIF-8 can be easily adjusted by changing the dosage of competing ligands and the reaction temperature. When the molar ratio of zinc acetylacetonate, 2-methylimidazole, and 2-butyl-1H-imidazole was 1 : 1 : 6, the HP-ZIF-8 with micropores (1.7 nm) and mesopores (3.9–30 nm) was synthesized at 50 °C and 30 MPa for 3 hours with excellent reproducibility. The as-synthesized ZIF-8 shows a high activity for CO2 adsorption, and the CO2 equilibrium adsorption capacity reached up to 1.49 mmol g−1 sorbent at 25 °C and 0.1 MPa. Moreover, the CO2 equilibrium adsorption capacity of HP-ZIF-8 was maintained at 1.36 mmol g−1 sorbent after 7 cycles.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Qin Wang,Xiaoyun Li,Huanting Li,Lijun Liu,Xu Zhang,Yanfang Li,Maoqing Kang,Qifeng Li,Junwei Wang
CO 2 -based poly(ether-carbonate) polyols (CO 2 -based PEC polyols), composed of carbonate and ether linkages, were synthesized by the copolymerization of CO 2 , chain transfer agent and propylene oxide (PO) in the presence of Zn–Co double metal cyanide (DMC) complex catalyst, and employed to prepare polyurethane elastomers (PUEs) successfully. To obtain high-quality poly(ether–carbonate) polyols, DMC catalysts were further modified by versatile low-molecule compounds and polymers including maleic acid, D-gluconate acid, ethylenediaminetetraacetic acid, polyacrylic acid, and polyacrylamide (PAM) as co-complexing agents (co-CAs). The catalysts bearing polymer co-CAs displayed much superior activity to those of low-molecule co-CAs counterparts. The best copolymerization activity was achieved by the DMC–PAM catalyst with a PO conversion of 86.9 % and a CO 2 incorporation of 23. 9 mol%. It was attributed to the low-symmetry crystal structure, high specific surface area, and strong acidity. Importantly, a conclusion concerning that N-containing polymers were highly effective co-CAs of the DMC catalysts was drawn. EXAFS analysis proved that various co-CAs caused changes in the coordination environment around Zn atoms. In addition, it was confirmed that the carbonate units in CO 2 -based polyols endowed PU−PEC with high tensile and tear strength, and strong water/toluene resistance, while the ether units in CO 2 -based polyols provided the advantages of high elongation at break, low viscosity, and low cost.
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高影响因子
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