JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.7
Hao Zeng,Xiangbing Zou,Shuo Yang,Sizhe Tang,Shanshan Luo,Meiyue Cheng,Haiping Xu,Yujie Song,Ming Liu,Yang Liu,Ming Yang,Bing Li
Functionalized cobalt phthalocyanine (CoPc) supported on carbon supports are promising electrocatalyst for the electrochemical reduction of carbon dioxide (eCO 2 RR), yet the role of functional groups on catalytic activity is pending for clarification and optimization to maximize the reaction kinetics. Herein, a series of eCO 2 RR catalysts are fabricated by affixing functionalized molecular catalysts onto the nitrogen-doped porous carbon (NPC), denoted as CoPc-4x@NPC (x = H, NH 2 and NO 2 ). Among them, CoTNPc@NPC exhibits exceptional eCO 2 RR performance: in an H-type cell, it achieves a current density of 45 mA cm −2 at −0.91 V vs. RHE with CO Faradaic efficiency (FE CO ) exceeding 93.5% over a wide potential range, long-term stability over 40 h, and a remarkable turnover frequency (TOF) of 23.49 s −1 . In a flow cell configuration, the CO partial current density ( J CO ) further increases to 224.1 mA cm −2 at −0.91 V. Density functional theory (DFT) calculations reveal that the nitro group upshifts the d -band center, enhances Co center electrophilicity, pre-donates electrons for *COOH formation, and underlies the higher turnover frequency. Integrating CoTNPc@NPC into a Zn-CO 2 battery delivers a maximum discharge power density of 3.86 mW cm −2 and stable operation for over 15 h. This work highlights the potential of molecularly engineered CoPc catalysts for eCO 2 RR and Zn-CO 2 battery applications, providing new insights for the rational design of high-performance electrocatalysts.
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高影响因子
Nano Research
·
2023
·Vol. 17
·期 5
·3684-3692
·
IF 9.9
Wu Wenbo,Zhu Jiaye,Tong Yun,Xiang Shuangfei,Chen Pengzuo
Regulating the electronic structure of Bi-based materials by alloying engineering is promising to promote the electrocatalytic activity, but it remains some challenges to be solved. In this study, a facile electrochemical co-deposition strategy is developed to synthesize the bimetallic Bi 9 Cu 1 alloy nanosheet on carbon cloth (Bi 9 Cu 1 /CC), which represents a novel self-supporting electrode for the electrocatalytic carbon dioxide (CO 2 ) reduction reaction (CO 2 RR). The Bi 9 Cu 1 /CC catalyst has achieved a remarkable catalytic performance with high Faradaic efficiencies (FE) of over 90% for formate at wide potentials from −0.7 to −1.2 V vs. reversible hydrogen electrode (RHE). Moreover, the reversible Zn-CO 2 battery can be driven by Bi 9 Cu 1 /CC cathode with a largest power density of 1.4 mW·cm −2 , and superior operating stability. The systematic characterizations and electrochemical results confirm that the improved catalytic active sites, the enhanced mass/charge transport and the optimal reaction kinetics of Bi nanosheet are realized for CO 2 RR by Cu alloying. In situ attenuated total reflection infrared (ATR-IR) result confirms the bimetallic Bi-Cu active sites prefer to follow the ⋆OCHO conversion pathway. The density functional theory (DFT) calculations suggest that the Cu alloying contributes to the increased density of states near the Fermi surface of Bi and the optimized adsorption of ⋆OCHO intermediates on the Bi sites, resulting in the excellent catalytic performance.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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LANGMUIR
·
2026
·Vol. 42
·期 31
·22950-22957
·
IF 4.4
Chen Nannan,Yuan Qingle,Liu Qin,Zhang Chao,Wu Zhengcui,Bi Wentuan
Single-atom catalysts (SACs) hold great promise for the
electrochemical
reduction of CO 2 to CO; however, the high selectivity is
typically restricted within a narrow potential window, limiting their
practical implementation. In this study, Ni–N–C catalysts
were supported on ordered and disordered carbon nanofiber membranes
(denoted as o-NiNC and d-NiNC, respectively) via electrospinning to
elucidate the effect of nanofiber alignment on CO 2 reduction
activity. The results demonstrate that o-NiNC catalysts allow for
spatially uniform H + /CO 2 delivery and consumption,
thereby mitigating the selectivity variations arising from uneven
spatial distribution of reactants. As a result, the o-NiNC catalysts
achieve a CO Faradaic efficiency (FE) of 98.5% at −1.0 V and
maintain an FE above 90% across a broad potential range (−0.6
to −1.6 V). This work provides new insights into the rational
design of high-performance CO 2 reduction electrocatalysts
through geometric engineering.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yang Chen,Pengfei Yan,Huanhuan Yang,Huan He,Huiwen Tian,Xueqi Liu,Jingjing Zhang,Huimin Lv,Wenzhuo Wu,Qun Xu,Buxing Han
Supercritical CO 2 works as a soft oxidant to adjust the oxidation states and crystal facets of Cu-based materials. • In the supercritical state, CO 2 dissociates to generate active *O on the Cu surface with water assistance. • Spontaneously reconstructed hydrogen bond network stabilizes the dissociated *O species for Cu oxidation to Cu 2 O {111}. • Ethanol induces thermodynamic selectivity towards Cu 2 O {110} facets via an interfacial adsorption coupling mechanism. • Facet-engineered Cu 2 O-Cu achieves over 73% Faradaic efficiency for CO 2 RR-to-syngas and a tunable CO/H 2 ratio of 0.25−0.94. Catalytic versatility of copper-based catalysts has been demonstrated to arise from synergistic effect between Cu and Cu 2 O with controlled crystal facets, though precise synthesis of crystal facet-tailored Cu-based catalysts remains challenging. Herein, we develop a novel strategy to partially convert Cu nanoparticles into crystallographically defined Cu 2 O with supercritical CO 2 (scCO 2 ) as soft oxidant. Under supercritical fluid state, CO 2 dissociation on Cu surface generates reactive ⁎ O species with assistance of water. The spontaneously reconstructed hydrogen bond network with surrounding water molecules stabilizes these dissociated ⁎ O species for Cu oxidation to Cu 2 O with exposure of {111} crystal facet. While, ethanol introduction induces the formation of Cu 2 O {110} rather than Cu 2 O {111} facet from a thermodynamic perspective through interfacial adsorption coupling. The resulting facet-engineered Cu 2 O-Cu catalysts exhibit excellent electrochemical CO 2 reduction reaction (CO 2 RR) for syngas production with a high Faradaic efficiency of >73% and a tunable CO/H 2 ratio of 0.25–0.94. The enhanced performance is attributed to the interfacial synergy between Cu and Cu 2 O with distinct crystal facets, which facilitates significantly improved electron transfer to the key ⁎ COOH intermediate and thus lowers the energy barrier for CO formation. This interfacial effect is particularly pronounced in Cu/Cu 2 O {110}. This scalable platform enables solvent-directed synthesis of surface-customized metal oxides for functional nanomaterials using scCO 2 as mild oxidant. Supercritical CO 2 dissociates to active ⁎ O species for Cu oxidation to Cu 2 O {111} with assistance of water, while ethanol introduction induces Cu 2 O {110} formation. The face-engineered Cu 2 O-Cu demonstrated enhanced CO 2 RR-to-syngas performance. Download: Download high-res image (92KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Haoran Sun,Chen Wang,Yucheng Liu,Mingming Yin,Shuo Wang,Lizhang Wang
To tackle the escalating problems of organic wastewater pollution and CO 2 emissions, we have developed a long-term operational electrocatalytic device for the one-pot electrochemical conversion of organic pollutants (using C 3 H 8 O 3 as a model compound) into liquid fuels. Commercial Pt/Ti and Sn served as the anode and cathode, respectively, with current density adjusted by varying the anolyte salt concentration. Experimental results show that the CO 2 proportion in the anode gas is low (<7 %), creating a “CO₂-depleted environment (2.6–6.6 % v/v )” in the cathode chamber. Surprisingly, formate can also be produced and the Carbon Utilization Efficiency (CUE) exceeds 80 %, despite the Faraday efficiency for formate (FE HCOO - ) consistently remaining below 2 % due to insufficient CO 2 supply from organic wastewater oxidation. While increased current density can boost CO 2 production, it concurrently exacerbates OH- accumulation, leading to a decrease in CUE, which necessitates finding an optimal balance between the two factors. Density functional theory (DFT) calculations reveal that increased CO 2 production in a “CO 2 -depleted” environment effectively enhances CO 2 adsorption energy on Sn and increases the reaction current density. This work reveals that the critical factor in enhancing FE HCOO - is identifying the optimal balance between anode CO₂ generation and cathode CO₂ utilization by adjusting current density, thus offering theoretical insights for targeted electrode fabrication and operational parameter optimization.
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Nanomaterials
·
2026
·Vol. 16
·期 8
·489
·
IF 4.8
Xin Peng,Lina Du,Gaoliang Fu,Shouren Zhang,Junying Ma
Photocatalytic reduction of carbon dioxide (CO2) into high-value multicarbon products, such as ethylene (C2H4), remains a significant challenge due to the difficult C-C coupling process. Potassium poly(heptazine imide) (K-PHI) is a promising photocatalyst, yet efficiently exchanging its interlayer cations to tune catalytic selectivity without causing structural degradation is difficult. Herein, an efficient and green supercritical CO2(SC CO2) assisted ion-exchange strategy was developed to successfully prepare a series of mono-/di-/trivalent cation-doped M-PHI photocatalysts (M = H+, Na+, Sr+, Ca2+, Co2+, Fe3+). Systematic characterizations confirmed that the SC-CO2treatment successfully achieved in-depth cation substitution without destroying the intrinsic heptazine framework, effectively regulating the interlayer structure and significantly optimizing the photoelectrochemical charge separation. Among the prepared samples, H-PHI exhibited the optimal photocatalytic CO2reduction performance with an outstanding selectivity toward C2H4generation. Under simulated sunlight irradiation for 3 h, the yields of CO, CH4, and C2H4C2H4C2H4reached 3564.87, 807.32, and 40.00 μmol·g−1, respectively, significantly outperforming pristine K-PHI and other metal-doped samples. Crucially, isotope-tracing experiments utilizing a SC CO2-DCl treatment detected deuterated CH4and C2H4products, providing direct evidence that the hydrogen in the carbon products originates from the introduced protons, thereby elucidating the precise reaction pathway for C-C coupling. This study provides a green and efficient supercritical CO2ion exchange strategy for the cation engineering of crystalline carbon nitride, and also offers new ideas and methods for designing high-activity photocatalysts for photocatalytic CO2reduction.
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ENERGY
·
2022
·
IF 8.857
Haorui Liu,Shuoyu Wang,Xiaoqiong Wang,XiaoJing Feng,Shuixia Chen
A novel stable porous solid amine adsorbent with three-dimensional interpenetrating network structure was prepared by polymerization of divinylbenzene using high internal phase emulsion (HIPE) template method , and followed by further introducing polyethyleneimine (PEI) by impregnation-crosslinking method. Fixed bed dynamic adsorption experiment proved that under wet condition, the former exhibited not only a higher capacity of 6.22 mmol/g but also a better adsorption kinetics process with faster adsorption rate and longer lag in breakthrough point, which makes it potential to be used in gas separation. In CO 2 /CH 4 separation experiment, PolyHIPE-PE30-4 showed a CO 2 /CH 4 separation selectivity of 253 at 298 K and 1 bar, and meanwhile exhibited an extra-high operating capacity. The pure methane productivity of PolyHIPE-PE30-4 was 24.1 mmol/g from CO 2 /CH 4 (80:20, v/v) mixed gas, 4.5 times to that of PE30-4 gel (5.36 mmol/g). Significantly, PolyHIPE-PE30-4 could maintain an excellent regeneration performance after at least 7 cycles, while PolyHIPE-P30 exhibited a remarkably decrease in adsorption capacity after only three adsorption-desorption process in wet condition, demonstrating the advantage of impregnation-crosslinking method for amine functionalization. The superior CO 2 adsorption capacity and regeneration stability, combined with its superior adsorption kinetics property make it a broad prospect in the field of CO 2 /CH 4 separation.
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FUEL
·
2021
·
IF 6.609
Xinjie Luo,Pengfei Zheng,Ke Gao,Bing Wei,Yujun Feng
Water-alternating-CO 2 gas (WAG) flooding is a common technique to enhance oil recovery via improving CO 2 sweep efficiency, but serious gas channeling may still occur, especially in reservoirs with strong heterogeneity, due to a poor blocking capacity of aqueous slugs to the “channeling” pathway induced by their low viscosity. Herein, a copolymer whose aqueous solution viscosity can be increased by both heat and CO 2 was developed and added into the aqueous slug to control gas channeling and increase oil recovery during enhanced WAG processes. The copolymer was synthesized by grafting poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) onto the triblock copolymer, Pluronic F127, PEO 100 -PPO 65 -PEO 100 . The aqueous copolymer solutions can be thickened/gelled by heating due to the formation of micelles as the physical cross-link and their entanglements even at a concentration as low as 0.2 wt%, and viscosified by bubbling CO 2 thanks to expanded copolymer coils caused by electrostatic repulsion-induced chain extension of protonated PDMAEMA chains. Notably, thermo- and CO 2 -triggered viscosifying can work synergistically and they are completely reversible upon cyclically heating/cooling the copolymer solutions and bubbling/removing CO 2 into/from the aqueous phase, respectively. In WAG flooding tests using two parallel cores, gas channeling was mitigated by blocking high-permeability cores due to in-situ thermo-induced gelation and CO 2 -triggered thickening of copolymer slugs, thus diverting chase fluids into unswept low-permeability cores and enhancing 21–22% total oil recovery than the conventional and HAPM-enhanced WAG modes. Importantly, owing to the characteristics of low initial viscosity, single component, and thermo-gelation, this dually-responsive copolymer possesses high injectivity and satisfactory gelation control. This work could enlighten the design of novel dual/multiple stimuli-thickening polymers used for channeling control and enhanced oil recovery.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Dan Li,Cuiping Li
A class of CO2-binding organic liquids (CO2-BOLs) composed of 1,1,3,3-Tetramethylguanidine (TMG) and Glycerol (Gly) and Gly’s amino derivatives were developed for highly efficient and reversible CO2 capture. These CO2-BOLs exhibited high gravimetric CO2 solubility up to 0.196 g CO2·g–1 at 313.2 K and 1.0 atm, superior to most functionalized ILs and other absorbents. The influential factors of CO2 absorption, such as components of CO2-BOLs, absorption temperature, and CO2 partial pressure together with water contents were investigated, and the recyclability of CO2-BOLs was verified to be excellent. The absorption mechanism of CO2-BOLs was explored with the help of spectral analysis, quantum chemical calculation, and thermodynamic analysis. All the results revealed that chemisorption took place once these CO2-BOLs were exposed to CO2, and alkyl guanidine carbonates were produced. Besides, it is illustrated that introducing the amino group to Gly could reduce the nucleophilic reactivity of CO2-BOLs, along with the absorption enthalpy simultaneously.
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APPLIED ENERGY
·
2018
·
IF 7.9
Xiaowen Zhang,Helei Liu,Zhiwu Liang,Raphael Idem,Paitoon Tontiwachwuthikul,Mohammed Jaber Al-Marri,Abdelbaki Benamor
The aim of this work is to find a potential way for great decrease in CO 2 capture energy requirement. Here, for the first time, a series of bifunctional Al 2 O 3 /HZSM-5 catalysts (Al-ZSM) were prepared by the combined precipitation ultrasound method and used for the CO 2 desorption process. All the investigated catalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrometry (FT-IR), N 2 adsorption–desorption, ammonia and CO 2 temperature programmed desorption (NH 3 /CO 2 -TPD) and pyridine-adsorption infrared spectroscopy (Py-IR). The regeneration behaviors of a 5 M monoethanolamine (MEA) solvent with four Al-ZSM catalysts were studied at an initial CO 2 loading of 0.5 mol CO 2 /mol amine and the temperature of 96 °C. The results reveal that all the catalysts improve the CO 2 desorption performance, the Al-ZSM catalysts show higher catalytic performance than the single catalysts Al 2 O 3 and HZSM-5, and the Al-ZSM can reduce the heat duty by 23.3–34.2% as compared with the catalyst-free test. The use of Al-ZSM in the MEA regeneration process improves the desorption performance by 2–3 times in comparison with the blank run. A possible dual sites mechanism of CO 2 desorption with Al-ZSM is suggested. The excellent performance of Al-ZSM can be attributed to their enhanced Brϕnsted acid sites (BAS), mesopore surface area (MSA) and basic sites, which resulted from the good synergistic reaction between the Al 2 O 3 and HZSM-5, and the base treatment for HZSM-5. Besides, the stability test of the Al-ZSM was conducted. Based on the results, the Al-ZSM demonstrate a superior catalytic performance for the rich amine regeneration process, and present an excellent cyclic stability, explicitly have the potential to be a promising industrial catalyst for CO 2 capture. Furthermore, the dual sites catalytic CO 2 desorption over bifunctional catalysts will open a new path to design better catalysts for the rich amine solution regeneration process to increase the desorption performance, reduce the regeneration energy consumption, and thus further decreasing the operation costs of CO 2 capture.
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APPLIED ENERGY
·
2018
·
IF 7.9
Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang
To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Daofei Lv,Renfeng Shi,Yongwei Chen,Yang Chen,Houxiao Wu,Xin Zhou,Hongxia Xi,Zhong Li,Qibin Xia
A water resistant zirconium–porphyrin metal–organic framework PCN-222 was synthesized for selectively separating CO2/CH4 and CO2/N2. Isotherms of CO2, CH4, and N2 on PCN-222 at low and high pressures were respectively measured. At 298 K, CO2 uptakes at 100 and 3000 kPa were 1.16 and 13.67 mmol/g, respectively. At 298 K and 100 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities separately reached 4.3 and 73.7. At 298 K and 3000 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities were 4.7 and 32.8, respectively. Importantly, breakthrough experiments confirmed that PCN-222 could achieve the effective separation of CO2/CH4 (both 50:50 and 10:90) and CO2/N2 (both 50:50 and 15:85) gas mixtures. The dynamic regeneration experiments showed that PCN-222 maintained its initial CO2 adsorption capacity after five cycles of CO2 adsorption–desorption. This work suggested that PCN-222 was a potential candidate for selectively separating CO2/N2 and CO2/CH4.
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