CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Nannan Liu,Qinglong Ru,Wei Jiang,Hui Hu,Yongcui Yang,Kailan Ma,Zuliang Du,Yu Jia,Xiaojing Yang,Bao Zhang,Gang Cheng
The sustainable development of human society is critically dependent on atmospheric CO 2 concentration. Herein, we have developed a catalyst-free CO 2 reduction approach that utilizes mechanical energy to drive gas–liquid triboelectric plasma, enabling the generation of CO and O 2 at room temperature and atmospheric pressure through regulating the decomposition pathway of CO 2 − radical anions. The reactivity of CO 2 − radical anions is predominantly governed by the state of gas-phase triboelectric plasma and the composition of liquid-phase solution. Under optimized reaction conditions, this system achieves a remarkable CO production rate of 20.7 μmol h −1 with nearly 100 % selectivity and an exceptional electrical-to-chemical energy efficiency of 71.2 %. The introduction of water and potassium ions significantly enhances the conversion of CO 2 − radical anions through the formation of hydrated CO 2 − intermediates. Isotope labeling experiments, control experiments, and theoretical calculations confirm that water molecules and alkali cations effectively stabilize the highly reactive CO 2 — radical anions through hydrogen bonding and electrostatic interactions, reducing the dissociation barrier from 3.46 eV for gas phase CO 2 — to 2.48 eV in the presence of K + ions. Furthermore, the mechanical energy-driven gas–liquid triboelectric plasma system demonstrates excellent compatibility with aqueous solutions commonly encountered in daily life, maintaining superior CO production activity across various aqueous environments. This gas–liquid triboelectric plasma approach for CO 2 conversion not only provides a promising strategy for greenhouse gas mitigation, but also offers fundamental insights and a new perspective on CO 2 fixation at gas–liquid interfaces.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xi Chen,Nana Wang,Guining Chen,Zhenggang Wang,Gongping Liu,Rongfei Zhou,Wanqin Jin
Mixed-matrix formulation is a promising method to overcome permeability-selectivity trade-off of polymers with incorporation of fillers with well-defined nanopores . The filler properties play a key role in determining the performance of mixed-matrix membrane (MMM). In this work, for the first time, we explored the critical effect of filler structural integrity on separation performance of MMM. Typically, micron as-synthesized, submicron as-synthesized and submicron ground SAPO-34 zeolites were incorporated into 6FDA-DAM polyimide , respectively. The interface compatibility between two phases was ensured by (3-aminopropyl) trimethoxysilane (APTMS) modification on SAPO-34 fillers. It was found that the directly synthesized micron and submicron fillers contributed to enhance the CO 2 /CH 4 separation performance whereas the submicron ground filler lowered the CO 2 permeability. Notably, incorporating 30 wt% micron as-synthesized SAPO-34 into 6FDA-DAM enhanced the CO 2 permeability by 68% and CO 2 /CH 4 by 37%, surpassing the performance upper-bound. Moreover, the hydrogen bonding between the filler and polymer matrix endowed the membrane with outstanding plasticization resistance with CO 2 partial pressure up to 20 bar. Adsorption isotherms and Maxwell model prediction revealed that the filler transport properties could be significantly affected by commonly-used methods of reducing the filler size. A decreased structural integrity was identified in the sequence of micron as-synthesized, submicron as-synthesized and submicron ground fillers. This work highlights the importance of a careful balance between structural integrity and crystal size of filler, and reliable routes to obtain nanofillers with desirable structural integrity as pursuing high-performing MMM toward practical application.
研究领域:
材料科学
·
化学工程
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ENERGY & FUELS
·
2025
·
IF 5.3
Yang Li,Xiaodong Shen,Xinlei Shi,Nanqin Zhou,Yinde Zhang,Bo Wang
Hydrate-based CO2 sequestration in submarine sediments is a promising large-scale carbon mitigation strategy. This study examined the effects of sediment grain size on CO2 hydrate formation kinetics, seepage behavior, and morphology evolution regulated by l-Methionine (l-Met) as a kinetic promoter, under controlled conditions of 3.6 MPa and 277.15 K, simulating the harsh environment of submarine organic-rich sediments. The experimental results demonstrate a nonunidirectional relationship between grain size reduction and sequestration enhancement. While finer sediments generally promote formation kinetics, the 98–138 μm quartz sand fraction exhibited optimal overall performance, achieving a CO2 consumption of 0.369 mol and the fastest growth rate (t90 = 58.027 min). This optimum reflects a balance between kinetic promotion and mass transfer, as evidenced by seepage tests showing that excessively fine sediments cause severe pore-throat clogging, leading to a marked reduction in effective permeability, whereas medium-grained systems exhibit the highest effective permeability. Mixed-grain systems display enhanced injectivity due to preferential flow pathways formed by coarse fractions. Visual observations reveal that CO2 hydrate in natural sea sands forms heterogeneously with nodular-like morphology. These findings offer theoretical guidance for optimizing kinetic promoter-regulated CO2 hydrate formation and continuous CO2 injection strategies in submarine sediments.
研究领域:
能源与燃料
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环境科学
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化学工程
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地球科学
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CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Ke Wang,Feng Gu,Peter T. Clough,Youwei Zhao,Pengfei Zhao,Edward J. Anthony
Lithium orthosilicate (Li 4 SiO 4 ) represents a potential class of high-temperature sorbents for CO 2 capture in power plants and sorption enhanced methane reforming to produce H 2 . However, conventional wisdom suggests that pure Li 4 SiO 4 should have extremely slow sorption kinetics at realistic low CO 2 concentrations. Here, we report the opposite result: using a simple and cost-effective glucose-based mild combustion procedure, an unusually efficient and pure form of Li 4 SiO 4 (MC-0.6) was synthesized to achieve a maximum uptake capacity of 35.0 wt% at 580 °C for CO 2 concentrations under 15 vol% and maintained this capacity over multiple cycles. The characterization results showed that highly porous nano-agglomerate-like (50–100 nm) morphologies were apparent and ensured a rapid surface-sorption of CO 2 . In this process, a macroporous nano-sized Li 2 SiO 3 cover on the melt layer of Li 2 CO 3 was identified for the first time. This special structure appeared to accelerate the transportation of CO 2 and the diffusion of Li + and O 2− through a molten layer enhancing contact with CO 2 . Thus, the sample MC-0.6 reduced both the surface-sorption and diffusion kinetics dependence on low CO 2 concentrations. Rather than use traditional approaches (controlled morphologies combined with doping), we have demonstrated that the slow kinetics can be overcome simply by a controlled morphologies strategy, which opens up a new direction for the synthesis of high-performance Li 4 SiO 4 sorbents.
研究领域:
材料科学
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环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Zhiwen Li,Jiari He,Zaiqi Li,Jia Song,Difei Xiao,Haixia Liu,Yuanyuan Liu,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang,Zeyan Wang
Pulsed electrocatalytic CO 2 reduction reaction (p-CO 2 RR) on copper-based catalysts can dynamically stabilize active Cu + sites and enrich surface *OH, enabling sustained CO 2 -to-C 2+ conversion. However, its practical application is still constrained by: 1) low time efficiency caused by both the inherent instability of Cu + during cathodic polarization and the sluggish re-oxidation of Cu 0 to Cu + , and 2) inadequate CO 2 -to-C 2+ conversion efficiency caused by the insufficient *OH coverage. To address these challenges, a Pd-modified Cu 2 O catalyst (Pd-Cu 2 O) with strong Pd-Cu electron interaction is designed. In situ experiments and theoretical studies reveal that Pd induces stable electron-deficient Cu + /Cu 0 sites, which effectively suppressing Cu + reduction during the cathodic phase and promoting Cu + regeneration during anodic phase, thus shortening the required oxidation duration. Concurrently, Pd accelerates water dissociation and enhances *OH coverage, which facilitates *CO adsorption and enhances C-C coupling. As a result, Pd-Cu 2 O achieves a Faradaic efficiency for C 2+ of 79.8 % with stable operation for over 50 h, and the time efficiency exceeding 87 %, outperforming most reported p-CO 2 RR catalysts. This work highlights the importance of rational catalyst design via electronic structure regulation for enhancing the time efficiency and C 2+ production performance for p-CO 2 RR, paving the way for efficient CO 2 -to-C 2+ conversion and practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Yutong Wang,Zili Fan,Menghan Yuan,Chenlin Zhang,Zihan Hu,Xinlin Cao,Xinming Zhou,Hui Fu
Biphasic absorbents are regarded as highly promising absorbents for carbon dioxide (CO 2 ) capture, owing to their potential energy savings and facile separation. This study introduces a novel piperazine (PZ)/2-(diethylamino)-ethanol (DEEA)/n-propanol (NPA) biphasic absorbent, in which the addition of NPA to the PZ/DEEA binary system results in a doubling of absorption rate, a reduction of the lower phase volume by over 50% to just 28.77% of the total volume, and a CO 2 enrichment level of up to 95.59%, achieving rich phase concentration. Furthermore, the PZ/DEEA/NPA absorbent exhibited excellent absorption-desorption stability and a high desorption efficiency (~ 90%), with a regeneration heat approximately 31% lower than that of benchmark monoethanolamine (MEA). NMR and molecular simulation analyses indicate that NPA's weak competitive solvation effect reduces dispersive interactions with CO 2 absorption products, thereby indirectly strengthening hydrogen bonding of products. This facilitates dense aggregation, resulting in a volumetrically contracted, high-concentration solid product during the final absorption stages. Additionally, corrosion assessments indicate that both fresh and CO 2 -saturated absorbents demonstrate extremely low corrosion rates, favoring industrial implementation. In conclusion, the PZ/DEEA/NPA biphasic absorbent proves to be a potential alternative to the conventional MEA for sustainable CO 2 capture.
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ENERGY & FUELS
·
2023
·
IF 5.3
Yanlin Liu,Jiren Tang,Yunzhong Jia,Yiyu Lu,Chenqing Shang,Rongrong Tian,Xiao Sun,Qi Cheng,Guilin Zhao
The surface wettability and morphology of shale may both be modified by SiO2 nanofluid (SNF), directly influencing the capillary force and CO2 geo-storage. However, the literature requires more information and studies with respect to nanoparticles’ effect on shale surface at reservoir conditions of high pressure and temperature. Here, we investigate the stability of nanoparticle layers formed by SNF on Longmaxi (marine) and Yanchang (continental) shale in ScCO2 and nanoparticles’ efficiency of wettability reversal at different nanofluid aging times and concentrations. Besides, low-pressure nitrogen gas adsorption (LP-NA) was performed to evaluate the effect of nanoparticles on shale pore structures after ScCO2 exposure. Results indicate that the nanoparticle structure could be stable in ScCO2 and render the wettability of shale samples to be more hydrophilic, while the quartz-rich Longmaxi shale surface shows a denser nanostructure than the clay-rich Yanchang shale surface does and presents a stronger water wettability. More micropores are transformed into mesopores or macropores for ScCO2- and SNF-treated Longmaxi samples than solely ScCO2 samples, but the pore structure parameters show trivial alteration in Yanchang samples after SNF treatment. The difference in the capillary force recovery between Longmaxi (recovered by 660.5%) and Yanchang (recovered by 500.6%) shale implies that silica nanofluid may be more suitable for Longmaxi formation in the CGS application.
研究领域:
石油工程
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碳捕集与封存（CCS）
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能源纳米技术
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储层地质学
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界面科学
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高影响因子
ACS Applied Polymer Materials
·
2026
·
IF 5.2
Ziyi Yuan,Zhihong Lin,Kejing Li,Jian Li,Viatcheslav Freger,Xuezhong He
Polymers of intrinsic microporosity (PIMs) are promising membrane materials for CO2 separation due to their high permeability; however, their limited CO2/N2 selectivity restricts practical application. Herein, mixed-matrix membranes (MMMs) were fabricated by incorporating a CO2-molecularly imprinted UiO-66-NH2 filler (MIP@U) into amidoxime-functionalized PIM-1 (AOPIM-1), followed by thermal treatment at 160 or 250 °C under vacuum to regulate the membrane microstructure. Spectroscopic and porosity analyses (FTIR, XRD, and N2 physisorption) show that thermal treatment at 160 °C promoted oxadiazole-ring formation, leading to enhanced subnanometer microporosity and improved CO2/N2 selectivity. In contrast, treatment at 250 °C partially regenerates nitrile groups and generates larger micropores, resulting in higher CO2 permeability but reduced selectivity. The MIP@U filler introduces CO2-recognition cavities and improves interfacial compatibility, enabling synergistic control of polymer microporosity and interfacial transport pathways. The optimized 3 wt % MIP@U/AOPIM-1-TR160 membrane achieves a CO2 permeability of ∼1600 Barrer and a CO2/N2 selectivity of 50.8. The membrane also demonstrates stable performance under pressures up to 12 bar and during 30 h of continuous operation at 2 bar. This study highlights a dual-approach strategy combining thermally tailored PIM chemistry with molecularly imprinted MOF fillers for designing high-performance MMMs for CO2 capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Cheng Gu,Yakun Qu,Ya Chen,Yunlong Wang,Chaowen Liu,Le Zhang,Xiangyang Cui,Xiaoguang Zhao,Enhui Xing,Yibin Luo,Zhen Chen,Junhua Li
Framework Fe-ZSM−5 was developed for catalytic CO 2 desorption from MEA. • Isolated tetrahedral Fe 3+ sites were incorporated into the MFI framework. • Framework Fe reduced Fe dissolution in MEA by more than 88% over 120 °C for 15 days. • Fe-ZSM−5 increased the average CO 2 desorption rate by 35% over the blank case under continuous operation. • Lewis acid-base pairs promote H 2 O-assisted carbamate decomposition. Catalytic CO 2 desorption from aqueous amine solvent is a promising strategy for energy-saving CO 2 capture from industrial flue gas. As an important candidate, conventional zeolite catalysts often suffer from insufficient activity, while metal incorporation can effectively regulate acidity but also causes metal-site dissolution. Herein, we prepared an excellent ZSM-5 zeolite with framework-incorporated Fe (Fe-ZSM−5) through feasible hydrothermal method. The coordination characterizations confirm that Fe-ZSM−5 contains isolated, tetrahedrally coordinated Fe 3 + within the MFI framework. Compared to impregnated Fe, the dissolution rate of framework Fe species in ethanolamine absorbent was reduced by more than 88%, which can effectively enhance catalytic performance and simultaneously avoid solvent degradation. Meanwhile, the incorporation of framework Fe modifies the acidic environment of the zeolite by generating Si-OH-Fe Brønsted acid sites and Fe-related Lewis acid sites. Fe-ZSM−5 exhibited high catalytic activity for CO 2 -rich MEA solution, with a peak desorption rate of 4.306 mmol·min −1 (48% higher than the blank case); the catalytic rate constants reach 2.0–2.4 × 10 −4 min −1 . This work proposes a novel design strategy for high-performance acid catalysts, representing a durable and efficient catalyst for reducing regeneration energy in amine-based CO 2 capture. Download: Download high-res image (299KB) Download: Download full-size image
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 35
·20723-20730
·
IF 4.6
Cong Shenzhen,Sun Si,Wang Ming,Zhang Yijing,Shen Qin,Zhang Yatao,Pang Huan
Membrane-based separation technology holds great promise
for CO 2 capture, yet conventional membranes are often constrained
by the permeability-selectivity trade-off. In this study, we developed
a zirconium-cluster (Zr 6 )-incorporated ZIF-8 membrane via
an electrochemical synthesis strategy to address this limitation.
The resulting Zr 6 @ZIF-8 composite membrane exhibits high
crystallinity, a dense microstructure, and homogeneous dispersion
of Zr 6 clusters within the ZIF-8 framework. The optimized
Zr 6 @ZIF-8–2 membrane demonstrates outstanding CO 2 separation performance with a CO 2 permeance of
up to 300.0 gas permeation unit and CO 2 /N 2 and
CO 2 /CH 4 selectivities of 27.0 and 14.8, respectively.
The Zr 6 clusters enable effective structural regulation
of ZIF-8 membranes, resulting in enhanced CO 2 separation
performance and leading to improved diffusion selectivity. Furthermore,
the membrane shows a stable separation performance under varying feed
pressures and temperatures, along with excellent long-term operational
stability. This work provides an effective electrochemical approach
for fabricating high-performance MOF-based membranes, offering a promising
candidate for industrial CO 2 capture and natural-gas purification.
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PubMed
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Chenhao Wang,Xiaoyun Miao,Ting Luo,Xingzhi Zhu,Xiaofeng Ye,Zhaoyin Wen
CO 2 hydrogenation using protonic ceramic electrolysis cells (PCECs) to produce fuel gases such as CH 4 and CO has been considered as a promising technology for effective CO 2 utilization. However, the long-term stability of conventional PCECs based on Y and Yb doped BaZrO 3 -BaCeO 3 (BCZYYb) proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO 2 . In this work, a new type PCEC based on CO 2 -tolerant La 5.6 WO 11.4−δ (LWO) material is firstly constructed. A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing, dip-coating and co-sintering process, followed by Ni and La 0.6 Sr 0.4 CoO 3−δ (LSC) catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO 2 hydrogenation reactor. Benefits from the synergistic catalysis of nano nickel and LWO, the reactor gets a CH 4 selectivity of over 50 % at 600 °C under 20 % CO 2 concentration, and it operates stably for over 320 h at 600–650 °C under high CO 2 concentrations of 50–80 %, showing no degradation in CO 2 conversion rate or CH 4 selectivity. Post-mortem analysis demonstrates that the CO 2 absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO 2 methanation. This study provides a viable strategy for designing highly stable PCEC-based CO 2 hydrogenation reactors.
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MOLECULES
·
2026
·Vol. 31
·期 3
·514
·
IF 5.1
Xiangjuan Meng,Mingwei Zhao,Zhenfeng Ma,Xinjie Xu,Zhongzheng Xu,Yuxin Xie,Yining Wu,Ziyi Wang,Wenhao Ren,Huan Zhang
CO2flooding is an effective technique for enhancing oil recovery in low-permeability reservoirs. However, it is often hindered by severe CO2channeling. This challenge is particularly pronounced in near-wellbore regions with large pressure differentials and in fractured reservoirs, where high CO2injection rates and rapid breakthrough require channel blocking systems with high mechanical strength and excellent CO2-resistant performance. In this work, a smart responsive polymer was synthesized and subsequently crosslinked with a highly active phenolic resin crosslinking agent to develop a smart responsive polymer gel channel blocking system. The resulting gel exhibits CO2-responsive strength enhancement and excellent CO2-resistant performance. The static and dynamic gelation behaviors, nonlinear rheological properties, CO2-resistant performance, channel blocking, and enhanced oil recovery performance of the smart responsive polymer gel were systematically investigated. The results demonstrate that the polymer gel maintains good structural stability during dynamic transport in the reservoir and does not undergo significant strength degradation under shear conditions. Moreover, the smart responsive polymer gel exhibits excellent CO2-resistant performance within a temperature range of 80–110 °C, salinity up to 10 × 104mg/L, and pressure up to 20 MPa. Moreover, the system shows a significant enhancement in channel blocking and enhanced oil recovery performance, highlighting its promising potential for effective CO2flooding channel blocking in low-permeability reservoirs.
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