JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Bingyuan Dai,Minxuan Wang,Hui Xu,Hongbing Zheng,Yongzheng Zhang,Cheng Ma,Jitong Wang,Wenming Qiao,Licheng Ling
The precise atomic-scale preparation of single-atomic active sites with unique coordination structures in electrocatalysts for the carbon dioxide reduction reaction (CO 2 RR), coupled with the elucidation of their mechanisms at the atomic level, remains a formidable challenge. In this manuscript, a simple one-pot synthesis method was adopted to successfully synthesize an O-doped Ni single-atom catalyst (Ni-NOG), characterized by a distinct Ni-N 2 O 2 symmetric coordination structure. The incorporation of Ni-O bonds alters the electronic configuration of the catalyst’s central atoms within the catalyst, thereby boosting both the catalytic selectivity and efficiency during CO 2 RR. The synthesized electrocatalyst exhibited outstanding performance in the CO 2 RR process, achieving a Faraday efficiency (FE) of 97.4 % at a potential of −0.8315 V versus to reversible hydrogen electrode (vs. RHE). Furthermore, the selectivity remained consistently above 95 % throughout a 98-hour stability test, surpassing the performance of most advanced catalysts currently available. Theoretical simulations demonstrate that the Ni-N 2 O 2 symmetric coordination structure shows a small activation barrier in the rate-limiting step, favoring the swift generation of intermediate species and demonstrating robust catalytic activity. This work not only offers a straightforward and approach method for the preparation of single-atom catalysts but also clarifies the pivotal role of O-element doping within the coordination environment in enhancing catalyst performance.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Longyun Zhang,Ganghua Zhou,Gaoran Chen,Heming Wang,Qian Zhao,Weiqin Yin,Jianjian Yi,Xingwang Zhu,Xiaozhi Wang,Xin Ning
The metal–organic frameworks (MOFs) rich in porous structures and their derivatives have been widely developed and applied to heavy metal adsorption. However, little attention has been paid to the subsequent treatment and reutilization of spent MOFs adsorbents. A potential feasible strategy is to develop MOFs-derived bimetallic catalysts for energy conversion. Herein, a bimetallic Ni-Cu 2 O-Cu/C nanocomposite (Ni-Cu/C) derived from spent Cu-based MOFs (CuBTC) adsorbents was fabricated and applied to improve the performance of photocatalytic CO 2 reduction. The results demonstrate that Ni doping could improve the charge transfer dynamics. The synthesized Ni-Cu/C catalyst exhibits a high CO yield (12.45 μmol g −1 h −1 ) in the pure water system in the absence of other photosensitizers and sacrificial agents, which is 2.05 folds higher compared to Cu/C. The CO 2 conversion selectivity of the synthesized Ni-Cu/C catalyst reaches up to 99.0%. The mechanism of photocatalytic CO 2 reduction reaction was further investigated by in-situ experiments and density functional theory calculation. The in-situ FT-IR characterization show that photogenerated electrons could effectively adsorb CO 2 to produce CO 2 − and optimize *CO immediate. This work not only emphasizes the unique design of bimetallic catalyst derived from spent MOFs adsorbent, but also contributes a feasible solution to its reutilization for enhanced CO 2 conversion.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2012
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IF 2.237
Jun Li,Chenjia You,Lifang Chen,Yinmei Ye,Zhiwen Qi,Kai Sundmacher
To reduce the high energy consumption and equipment corrosion in conventional processes of CO2 capture with aqueous amine solutions, the mixed nonaqueous solvents of monoethanolamine (MEA), diethanolamine (DEA), and diglycolamine (DGA) with polyethylene glycol (PEG) as cosolvent were explored for CO2 capture. The dynamic experiments of CO2 absorption and desorption were carried out to evaluate the performance of the studied nonaqueous solutions. It demonstrated that the mixed solutions of amines and PEG exhibited higher CO2 cyclic capacity and regeneration efficiency compared with the only aqueous amine solutions. Especially, the solution of 3 mol/L DGA-PEG200 exhibits a high cyclic capacity of 0.438 mol CO2/mol DGA and a high regeneration efficiency of 94.6%, which indicates its great potential in industrial application. Moreover, the very low vapor pressure of PEG helps the mixed solution for CO2 capture with reduced corrosion, energy consumption, and environmental pollution.
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LANGMUIR
·
2025
·
IF 3.9
Yuchen Zhou,Zezhi Chen,Huijuan Gong,Donglin Jiang,Huiqiang Yu,Lu Chen
Zinc porphyrin is a promising carbonic anhydrase (CA) mimic for promoting CO2 absorption, but its application is hindered by poor dispersibility in absorption solutions. To address these challenges, we developed a strategy to impregnate zinc porphyrin on an γ-Al2O3 carrier. The hydrophilic surface groups and porous structure of γ-Al2O3 were expected to enhance both the hydrophilicity and stability of zinc porphyrin. To verify its feasibility, zinc tetraphenylporphyrin (ZnTPP) was chosen as the representative to synthesize ZnTPP/Al2O3. Characterizations showed that ZnTPP could be loaded into the pores of γ-Al2O3 in a highly dispersed state. Also, ZnTPP/Al2O3 could be uniformly dispersed in the absorption liquid, effectively exposing the Zn2+ active sites and reducing diffusion resistance. CO2 absorption experiments revealed that ZnTPP/Al2O3 significantly enhanced CO2 absorption in water, 20 wt % K2CO3, and 20 wt % monoethanolamine (MEA) solutions, far outperforming original ZnTPP. Density functional theory (DFT) calculations further elucidated the interaction mechanisms, showing that oxygen atoms on γ-Al2O3 stabilize ZnTPP by forming van der Waals and coordination bonds with Zn2+ active sites. Additionally, these oxygen atoms donate electrons to Zn2+, enhancing its catalytic activity. These findings highlight the effectiveness of this strategy and provide a promising pathway for optimizing other CA-mimics for CO2 capture applications.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Wenxing Ye,Yizhen Tang,Xiaoru Liang,Qingyuan Luo,Weihai Liang,Chao Chen,Ke Zhang
Porous silicas have been extensively investigated as amine carriers for the production of CO 2 adsorbents, while few studies demonstrated that as-synthesized silicas (without template removal) can also serve as good amine carriers for efficient CO 2 capture. This raises a fundamental question of whether the time-consuming and energy-intensive process of removing the template from as-synthesized silicas is still necessary. More importantly, a reasonable mechanism is quite needed to explain the as-synthesized silicas as effective amine carriers. To this end, in this study, four types of as-synthesized silicas were compared together with their corresponding porous silicas as amine carriers for CO 2 capture. Experimental results show that as-synthesized silicas exhibit comparable or even better performance at medium amine loadings (50 ∼ 60 wt%), including larger CO 2 adsorption capacities and better cyclic stability, while porous silicas predominate at high amine loadings (70 wt%). Molecular simulation results indicate that the amine species are located in the interparticle cavities in the silicas rather than in the structural pores. This work provides important guidance for the future design of practical solid-amine CO 2 adsorbents.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Kunpeng Hou,Hairong Wu,Guorui Xu,Genglin Li,Tianfang Luan,Jiawei Chang,Tong Cheng,Zhaojie Song,Jirui Hou
Aiming to address the issues of limited suitability of conventional chemical oil displacement materials for formation conditions and the serious emulsification of oil and water in the produced liquid, the innovative nano oil-displacing system with CO 2 -responsive behavior has been developed. This system integrates oil displacement and emulsion breaking. The efficacy of the CO 2 -response system in creating stable emulsions with a high capacity to decrease interfacial tension has been demonstrated. The interfacial responsive behavior of all active components, including Janus nanoparticles, sodium oleate, gums, and asphaltenes, in the emulsion system was analyzed in terms of interfacial rheology and adsorption. Additionally, the prepared system demonstrated a rapid response to CO 2 , effectively breaking the emulsion within 5 min. Furthermore, the oil recovery enhancing mechanism of the CO 2 -response system was investigated using a microscopic visualization model. The system was proved to be efficient in initiating the residual oil within pore channels. Considering the combined effectiveness of the CO 2 -response system in terms of efficient oil displacement and rapid response, it offers valuable insights for advancing the chemical flooding technology of in enhanced oil recovery.
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Nano Research
·
2024
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IF 9.5
Zhang Guiru,Ji Ning,Lyu Shiheng,Ni Baoxin,Shen Peng,Ye Ke,Wang Yuting,Jiang Xuheng,Zhang Hai,Liu Xi,Wang Yongcheng,Jiang Kun
Electrochemically converting CO 2 into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions, yet largely limited to short-chained C 1 –C 3 products. Herein, we demonstrate a tandem artificial synthesis of biodegradable polyhydroxybutyrate (PHB) plastic from CO 2 building blocks. Batch synthesis of defects-enriched Bi catalyst is firstly demonstrated by plasma bombardment and following in situ electrochemical reduction, which delivers a HCOOH Faradaic efficiency above 80% at tunable concentration from 2 to 250 mM, an energy efficiency up to 41%, and a single-pass carbon conversion efficiency up to 60%. Annular dark field and second electron microscopic analysis, density functional theory (DFT) calcualtions, coupled with H-type and solid-state electrolyzer assessments, point out the vital role of defective and/or stepped Bi surface sites in promoting CO 2 -to-HCOOH conversion. Thereafter, as-synthesized high-purity HCOOH is used as the sole carbon source for C-chain growth within microbial fermentation reactor with Ralstonia eutropha , where activated formate dehydrogenase and increased metabolites related to Calvin–Benson–Bassham cycle are found to be responsible for the enhanced polyester accumulation.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Xianwei Fu,Ziyu Ma,Luoyu Liu,Sajjad Hussain,Qiuye Li,Dongwei Ma,Shilong Jiao
Electrochemical conversion of carbon dioxide into formic acid, which is one of the most economically viable chemicals, has been demonstrated as an efficient approach for closing the carbon cycle. However, it’s still challenging to reduce the overpotentials and increase the current densities for the future deployment of the CO 2 electrolysis technology. Here, we boost the intrinsic activity of the Bi-based electrocatalyst through the synergy of the enhanced charge transfer and mass transport process in the electrochemical reactions by generating an atomic disorder in the crystal lattices. The amorphous Bi-based quantum dots (a-BiQDs) serve as promising electrocatalysts toward formate production in a wide potential range with high Faradaic efficiency ( FE ) and energy efficiency ( EE ) in both the conventional H-cell and flow-cell, which is almost 5-fold enhanced in comparison with its crystalline counterpart. The maximum FEs of 94.44 % and 98.89 % are achieved at the potential of −1.0 V vs. RHE in the H-cell and flow-cell, respectively. Furthermore, long-term stability of more than 900 h is demonstrated in a two-electrode configuration. Combined molecular dynamics and first-principle calculations ascribe the remarkable activity toward formate production to synergistically accelerated mass transport and charge transfer kinetics during the electrocatalytic process. This work provides an effective approach for constructing electrocatalysts with high intrinsic activity, desired selectivity, and sufficient durability for large-scale deployment of CO 2 electrolysis technology.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Wenhui Li,Xiaowa Nie,Xiao Jiang,Anfeng Zhang,Fanshu Ding,Min Liu,Zhongmin Liu,Xinwen Guo,Chunshan Song
Screening of various supports reveals that Co catalysts supported on ZrO 2 and Al 2 O 3 show good initial activity for CO 2 methanation. Co/ZrO 2 and Co/Al 2 O 3 catalysts prepared by impregnation with different metal loadings were further examined comparatively. The 10Co/ZrO 2 catalyst showed high activity with CO 2 conversion of 92.5% and CH 4 selectivity of 99.9% without deactivation after 300 h time on stream (TOS). However, the 10Co/Al 2 O 3 catalyst gave a lower CO 2 conversion of 77.8% which decreased to 38.6% after 300 h TOS. The catalysts were characterized by STEM/EDS (scanning transmission electron microscopy/energy-dispersive X-ray spectroscopy), in situ XRD(X-ray diffractometer), H 2 -TPR(temperature programmed reduction), XPS (X-ray photoelectron spectroscopy), chemisorption of H 2 , CO, CH 4 , CO 2 and NH 3 -TPD (temperature programmed desorption). Re-dispersion of Co species on the ZrO 2 support during reduction by H 2 was observed by STEM/EDS. New Co-Zr phase formed on the Co-ZrO 2 interface was directly observed by TEM for the first time; the Co/ZrO 2 catalyst exhibited high stability with high activity for CO 2 conversion. In situ XRD, H 2 -TPR and XPS results indicate the promoting effect of ZrO 2 on the reduction of Co 3 O 4 to Co metal along with the negative effect of Al 2 O 3 . The oxygen vacancies on the ZrO 2 detected by XPS may help to activate CO 2 and H 2 O and resist deactivation. Co/Al 2 O 3 catalyst deactivates rapidly due to coke deposition and spinel formation.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 37
·19954-19962
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IF 8.867
Yiming Zhang,Huixian Wang,Jindun Liu,Jingwei Hou,Yatao Zhang
In this work, carbonic anhydrase (CA) molecules were embedded into metal–organic frameworks (MOFs) via physical absorption and chemical bonds, which could overcome the enzymatic inactivation and the poor separation property of pristine MOF materials. And then, these nanocomposites (enzyme-embedded MOFs) as the crystal seeds were in situ grown on oriented halloysite nanotube layers to develop novel biocatalytic composite membranes. These membranes exhibited optimal separation performance with a CO2/N2 selectivity of 165.5, about 20.9 fold higher than that of the membrane without embedded CA molecules, surpassing the Robeson upper bound (2008). At the same time, the CO2 permeance increased about 3.2 fold (from 7.6 GPU to 24.16 GPU). Importantly, the biocatalytic composite membranes showed good stability and mechanical properties and were easily scalable, which could be extended to industrial applications.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Siyao Wang,Jingfa Zhang,Yongchao Sun,Fangxu Fan,Qizheng Zhao,Gaohong He,Canghai Ma
Thermally rearranged (TR) polymers are increasingly pivotal in gas separation membranes, with a pressing need for advancements in mechanical strength and separation performance. In this work, a novel variety of TR polymers were synthesized by polymerizing an amine-functionalized triptycene structure with thermally rearrangeable ortho -hydroxy groups. The TR membranes demonstrate enhanced gas permeability in H 2 /CH 4 and CO 2 /CH 4 tests and increased polymer chain spacing. Additionally, incorporating triptycene enhanced the mechanical properties of TR polymers, primarily attributed to the π-π stacking interactions of the triptycene units. Notably, the 6FDA-BAP:DAT (2:1) membrane thermally rearranged at 400 °C exhibited a H 2 permeability of 225.3 Barrer and a H 2 /CH 4 selectivity of 146.3, representing increases of 320 % and 154 %, respectively, compared to the precursor, and surpassing the H 2 /CH 4 upper bound. This work presents a robust design strategy for preparing mechanically durable TR membranes with enhanced gas separation performance.
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