CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Longmei Li,Feiyang Hu,Xiuxing Cai,Tingrui Zeng,Qing Liu,Runping Ye,Lei Gong,Rongbin Zhang,Gang Feng
Uniformly dispersed and confined hm-Ni/CeO 2 catalysts were synthesized for CO 2 hydrogenation. • The hm-Ni/CeO 2 outperforms its mesoporous counterpart, reaching 84.56% CO 2 conversion at 325 °C with good stability. • The hm-Ni/CeO 2 possesses abundant oxygen vacancies and a higher Ni distribution. • In-situ DRIFTS and DFT studies confirmed that the enhanced methanation performance originates from oxygen vacancies promoting the formate pathway. Confined structure catalysts are widely dedicated to boosting catalytic activity and stability , while controlling their micro-environment and intermediate species remains a challenge. Herein, mesoporous (m-Ni/CeO 2 ) and hollow mesoporous (hm-Ni/CeO 2 ) catalysts were prepared via electrospinning and evaluated for CO 2 hydrogenation to methane. The hm-Ni/CeO 2 catalyst exhibits superior performance, achieving 84.56% CO 2 conversion at 325 °C, along with enhanced low-temperature activity compared to the m-Ni/CeO 2 catalyst. Characterizations revealed that the hm-Ni/CeO 2 catalyst possesses a higher oxygen vacancies and improved Ni dispersion, thereby enhancing metal-support interaction. Furthermore, synchrotron radiation and in-situ DRIFTS confirmed that the hm-Ni/CeO 2 catalyst facilitates the formation of bridging bidentate formate intermediates, which are more favorable for CH 4 production. Finally, DFT verified the predominance of the formate pathway and revealed that oxygen vacancies substantially enhance the reactivity of CO 2 methanation. This work not only develops a novel synthetic strategy for confined porous catalysts but also provides fundamental insights into the role of oxygen vacancies in CO 2 hydrogenation. Download: Download high-res image (203KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Zhuobin Mo,Wenfei Long,Yutian Zhang,Ningce Zhang,Jiale Sun,Shuxuan Liu,Shuai Chen,Haiqi Liang,Chao Liu,Luyao Ma,Shengnan Liu,Bohua Ren,Shuangyin Wang,Guobin Wen
Electrochemical CO 2 reduction to CO represents a promising avenue for generating value-added chemicals and achieving global carbon neutrality. However, mass transport plays a significant role in the expression of catalytic intrinsic activity which further restricts the selectivity promotions. Herein, we engineered a grooved electrode to enhance mass transport of dissolved CO 2 in the batch cell, inspired by the chimney effect, a phenomenon that drives the diffusion of species from high-concentration to low-concentration regions via the concentration gradient in the vertical direction. This structure enhances the diffusion depth of reactants within the catalyst layer by increasing the vertical concentration gradient, thereby effectively reducing CO 2 dead zones in the electrode. Through multiphysics modeling, we optimized groove geometry, creating a special grooved electrode that that further reduces CO 2 dead zones. Comparative analysis revealed that increasing the catalyst loading to 20% resulted in CO Faradaic Efficiency improvements of 26% for parallel-grooved electrodes, and 50% for special-grooved electrodes, significantly improving CO conversion in H-cell reactors. And in flow cell tests, the special-grooved electrode maintained a FE CO of 81% at a current density of 150 mA cm −2 , outperforming the other two electrodes.
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Journal of Physical Chemistry C
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2026
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IF 3.4
Tianyu Tang,Guowei Wang,Yitong Wang,Xin Jiang,Zhijun Li,Cailing Chen,Ziqing Zhang,Liqiang Jing
Poly(heptazine imide) (PHI) has garnered significant attention as a promising material for photocatalytic CO2 reduction. However, its practical application is hindered by limitations stemming from inefficient electron-mediated reduction processes and sluggish hole-driven oxidation kinetics. Herein, the Ni single atoms and hollow CoFe Prussian blue analogs were precisely decorated on PHI (CoFePBA@Ni-PHI) through a two-step calcination and in situ ion exchange-growth conversion process. The optimized CoFePBA@Ni-PHI photocatalyst demonstrates a superior CO evolution rate of 41.3 μmol g–1 h–1 in pure water without sacrificial agents, representing a 4.5-fold and 5.7-fold enhancement compared to pristine PHI and g-C3N4, respectively. The enhanced photocatalytic performance is primarily ascribed to the synergistic redox dual-site modification, where Ni single atoms serve as electron extractors to promote CO2 reduction, while hollow CoFePBA functions as hole-trapping sites to facilitate water oxidation, thereby collectively accelerating the overall photocatalytic process. This work elucidates the critical role of dual redox site engineering in photocatalytic systems and provides a rational design strategy for constructing efficient photocatalysts toward solar-driven fuel production.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Yiqin Zhang,Ruoxuan Peng,Hongyang Zhang,Shengnan Lan,Jiancheng Zhou,Naixu Li
The intense photothermal coupling effect generated by concentrating light through Fresnel lenses can efficiently convert CO2 into high-value-added chemicals. However, the extreme high-temperature environment resulting from high photon flux simultaneously causes the agglomeration, sintering, and oxidative deactivation of catalyst powders, thereby limiting the large-scale application of concentrated photocatalytic technology. Here, we constructed a high-temperature-resistant monolithic catalyst by in situ growth of NiO/WO3 nanosheets on the surface of the silica–alumina fiber material (denoted as NiO/WO3/SAF) and applied it to concentrated solar-driven CO2–H2O catalytic conversion. During the concentrated photocatalytic process, NiO/WO3/SAF exhibited superior cycling stability compared to NiO/WO3 powder, which could be attributed to the excellent dispersion, stable anchoring, and thermal insulation effects provided by the SAF support for NiO/WO3. Furthermore, under the assistance of oxygen vacancy-induced photothermal effect in WO3, the high-energy and high-density charge carriers generated by concentrated light facilitated CO2 reduction at electron-rich NiO active sites. Consequently, under concentrated irradiation of 4.0 W·cm–2, NiO/WO3/SAF achieved a solar-to-chemical energy conversion efficiency of 0.37‰, with CO and CH4 yields of 461.7 μmol·g–1·h–1 and 125.7 μmol·g–1·h–1, respectively. This work provides a valuable strategy for the industrial development of solar-driven CO2 utilization.
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高影响因子
CATALYSIS LETTERS
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2026
·Vol. 156
·期 6
·156
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IF 2.5
Tao Kun,Zhao Chao,Yu Wenya,Hu Shengye,Xue Hui,Zhang Mengmeng M.
Converting CO 2 into valuable chemicals is a sustainable way to address the energy and environmental crisis, yet achieving high selectivity toward CO remains challenging. Here, a S-doped copper-bismuth oxide (S-CuBiO x ) catalyst with a hierarchical structure was synthesized via a facile solution method toward selectively producing CO from CO 2 . The prepared S-CuBiO x exhibits a 91.3% CO Faradic efficiency at −0.9 V RHE in an H-type cell with 0.5 M KHCO 3 solution, delivering a 3.8-fold enhancement compared to the undoped CuBiO x , while decreasing the H 2 and HCOOH by-products to 2.6% and 4.5%, respectively. The doped-S can be responsible for the excellent CO selectivity, namely, the S dopant induces S-M-O (M = Cu or Bi) bond formation and tunes the local electronic structure of S-CuBiO x , thus benefiting *COOH formation/stabilization and accelerating the reaction kinetics toward CO. This work provides a rational design strategy for steering CO 2 RR selectivity toward CO via non-metal heteroatom doping in bimetallic oxide systems. Graphical The alternative text for this image may have been generated using AI.
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Advanced Energy Materials
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2026
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IF 25.5
Zhaorui Kong,Xinyi Wan,Meng Li,Bin Hua
Controlling the dynamic reconstruction of oxide-derived catalysts is critical for electrochemical CO 2 reduction because their active structures are often metastable under cathodic conditions. For SnO 2 -based catalysts, partial reduction generates reconstructed SnO 2 /Sn interfacial structures that favor formate production, whereas excessive reduction to metallic Sn destroys these interfaces and promotes hydrogen evolution. Here, we develop a dopant-regulated reconstruction strategy in which low-valence, high-electronegativity Bi acts as an electronic brake to modulate SnO 2 reduction kinetics. The optimized Bi0.2 catalyst delivers a formate Faradaic efficiency above 93% for more than 130 h at 250 mA cm −2 in a flow cell and maintains robust performance across diverse electrolyte environments. In situ and ex situ structural/electronic characterizations show that Bi incorporation mitigates deep SnO 2 reduction and helps preserve the reconstructed SnO 2 /Sn interface under cathodic operating conditions. In situ Raman spectroscopy and attenuated total reflection surface-enhanced infrared absorption spectroscopy measurements reveal potential-dependent changes in the interfacial water environment and support the involvement of activated CO 2 -related and * OCHO-related species in formate formation. Density functional theory calculations further show that Bi lowers the largest uphill Gibbs free-energy step for * OCHO formation while increasing that for the competing hydrogen evolution reaction pathway. These results establish dopant-regulated reconstruction and interfacial proton-coupled reaction regulation as design principles for sustainable CO 2 valorization.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Lei Shu,Dan-Dan Chen,Can Li,Yun-Lei Teng,Bao-Xia Dong
Covalent organic frameworks (COFs) incorporating metalloporphyrin units have gained significant attention as electrocatalysts for CO 2 reduction. However, conventional phenylporphyrin-based COFs are fundamentally limited by narrow pore sizes (<3 nm), which impose severe mass transfer resistance and impede catalytic turnover. Herein, we report a biphenyl porphyrin-based COF (DpPor-COF) with an expanded pore size of ∼3.8 nm, constructed from 5,10,15,20-tetra(4-formylbiphenyl)porphyrin and p -phenylenediamine. Subsequent metallation with Fe 3+ , Co 2+ , and Ni 2+ furnishes atomically dispersed M–N 4 sites (M-DpPor-COF), effectively suppressing metal leaching while expanding the electrochemical active surface area. Among the series, Co-DpPor-COF delivers a CO Faradaic efficiency (FE CO ) of 94% at −0.65 V vs. RHE with a high turnover frequency (TOF) of 477 h −1 , and maintains stable operation over 120 h. In situ infrared spectroscopy and DFT calculations reveal that transition metal centers lower the energy barrier for key intermediate steps in CO 2 -to-CO conversion, enhance charge density at the porphyrin core, and facilitate CO desorption. This work establishes a versatile strategy for concurrent pore engineering and active-site optimization, offering valuable insights for designing next-generation porous electrocatalysts. A biphenyl-porphyrin COF with an expanded 3.8 nm pore size is synthesized via the condensation of 5,10,15,20-tetra(4-formylbiphenyl)porphyrin and p -phenylenediamine, followed by metalation to introduce atomically dispersed M-N 4 sites, which delivers 94% CO Faradaic efficiency, 477 h −1 TOF and 120 h stability for efficient CO 2 electroreduction. Download: Download high-res image (175KB) Download: Download full-size image
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WASTE MANAGEMENT
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2026
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IF 7.3
Yunfeng Liu,Lu Yao,Xuechun Yang,Zheng Jiao,Nianci Guan
Li was fully extracted; Ni, Co and Mn recoveries exceeded 97 %. • 0.30 M ascorbic acid enabled leaching without additional reducing agents or heating. • Pressurized CO 2 enhanced ascorbic-acid leaching beyond physical pressurization. • Product-layer diffusion best described the overall leaching kinetics. • Leachate-derived NCM811 retained 150 mAh/g after 200 cycles. The recovery of critical metals from spent Ni–Co–Mn (NCM) cathodes commonly requires concentrated acids, auxiliary reductants, or energy-intensive treatment. Here, pressurized CO 2 –ascorbic acid leaching was integrated with leachate-based NCM811 regeneration. Under the optimized condition, 0.30 mol/L ascorbic acid, 7 MPa CO 2 , a solid-to-liquid ratio of 20 g/L, and 25 °C, Li was completely extracted within 80 min, while the extraction efficiencies of Ni, Co, and Mn reached 98.3 %, 97.1 %, and 97.2 %, respectively, without a separately added reducing agent. Control experiments confirmed that the increase in metal extraction arose from the coupled action of pressurized CO 2 and ascorbic acid rather than from physical pressurization or CO 2 alone. Equilibrium analysis further indicated that ascorbic acid provided the principal acidity and reducing capacity, while the dissolved CO 2 /H 2 CO 3 /HCO 3 – equilibrium can maintain protons availability during lattice dissolution. Kinetic fitting showed that the leaching behavior was best described by the product-layer diffusion model. SEM–EDS, XRD, and XPS revealed particle fragmentation, progressive disruption of layered structural order, and changes in surface valence states. The Li/Ni/Co/Mn-rich leachate was further converted into regenerated NCM811, which delivered discharge capacity of 180 mAh/g initially, retained 150 mAh/g after 200 cycles, and maintained 55–60 mAh/g at 5C. This approach achieves high metal extraction at room temperature using a relatively low organic-acid concentration without separately added reducing agent, while returning the recovered metals to functional cathode production. Download: Download high-res image (220KB) Download: Download full-size image
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Yingying Li,Guangyao Zhang,Deqi Fan,Zongze Li,Yi Lu
Achieving efficient and selective solar-driven CO2 reduction remains a grand challenge due to sluggish proton–electron transfer kinetics and limited reactant availability at catalytic interfaces. Herein, we present a hierarchically structured aerogel integrating triazine-based covalent organic frameworks (TCOF) with Nb2CTx MXene nanosheets embedded in a poly(vinyl alcohol)/sodium alginate (PVA/SA) matrix. The aerogel leverages broadband light harvesting, hierarchical water regulation, and localized photothermal activation to enhance multielectron CO2 conversion. The hydrophilic–hydrophobic PVA/SA scaffold promotes rapid water uptake and vapor-phase transport, while Nb2CTx enables efficient near-infrared-induced heating to establish a proton-rich interfacial microenvironment. Simultaneously, the porous TCOF network offers abundant CO2 adsorption and activation sites. This synergistic architecture facilitates stable proton-coupled electron transfer (PCET) pathways and C–C coupling. In situ spectroscopic analyses reveal enhanced formation and stabilization of *COOH, *CH3, and *OCCHO intermediates under photothermal conditions, evidencing facilitated C–C coupling for C2 product generation. Under 3-sun irradiation for 3 h, the optimized TCOF/Nb2CTx aerogel delivers exceptional yields of 119.3 μmol·g–1 CH4 and 94.9 μmol·g–1 C2H4, which is 2-fold higher than powder analogues and surpassing previous COF/MXene systems. This work demonstrates a generalizable strategy to engineer carbohydrate polymer-based aerogels with integrated light-to-heat conversion, vapor regulation, and catalytic site accessibility for efficient solar-to-chemical fuel generation.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yaqi Liu,Jie Jiang,Yun Ju,Jing He,Hong Zhang,Jing Zhao,Lina Qiao
Pyruvate, serving as a bridge between the linear acetyl coenzyme A (acetyl-CoA) and the reductive tricarboxylic acid (rTCA) cycle, is of prime importance for life evolution. However, the carboxylation of pyruvate with carbon dioxide (CO 2 ) followed by coupling into the rTCA cycle remains challenging in prebiotic chemistry. Here, we present that pyruvate spontaneously undergoes carboxylation with CO 2, giving oxaloacetate, malate, and fumarate of the rTCA cycle in water microdroplets at room temperature without catalysts. The current pathway that pyruvate directly uses CO 2 as a carbon source depends on the microdroplet surface, distinct from the previously reported pathway using glyoxylate. These findings suggested that pyruvate may have participated in the cycle of enzyme-free carbon fixation on a prebiotic Earth. Furthermore, the widespread microdroplets in the atmosphere may also have acted as a potential synthesis setting for CO 2 fixation and utilization. This offers a promising strategy for climate change control and the promotion of sustainable carbon cycling in the future.
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JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Jilei Lin,Meiqing Shen,Bowen Li,Gurong Shen,Yilin Wang,Xinhua Li,Liwei Jia,Feng Gao,Wei Li
The thermodynamic limitations of conventional propane dehydrogenation (PDH) have motivated the use of CO 2 as a mild oxidant to enhance reaction performance. However, on Pt-based catalysts that are renowned for their high C–H activation capacity, the introduction of CO 2 often leads to rapid catalyst deactivation. Here, we show that the primary cause of this deactivation is CO generated in situ via the reverse water–gas shift (RWGS) reaction. CO strongly adsorbs onto Pt active sites in PtIn/Al 2 O 3 , especially on isolated Pt atoms, with adsorption energies far exceeding those of propane. This preferential adsorption blocks propane from accessing active sites, suppressing dehydrogenation and reducing the number of available catalytic sites. Moreover, CO adsorption promotes Pt nanoparticle sintering, which increases coke deposition and facilitates side reactions, further accelerating deactivation. These findings provide mechanistic insights into the instability of Pt-based catalysts under CO 2 -assisted PDH (CO 2 -ODHP) and highlight the critical role of CO-induced surface effects in catalyst design and optimization.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xupeng Fu,Wei Tian,Yuting Wang,Xionghui Wei,Zhaojun Wu,Jianbin Zhang
The influence of water content on the physicochemical properties of the H 2 O + (polyethylene glycol 300 (PEG300) + hydroxyethyl ethylenediamine (AEEA)) mixed system was investigated in detail. Density ( ρ ) and viscosity ( η ) were systematically measured over the temperature range of 298.15 K to 318.15 K under atmospheric pressure, and electrical conductivity was determined at 298.15 K. Based on the experimental data, excess molar volume ( V m E ), excess Gibbs free energy of activation for viscous flow ( ΔG ⁎E ), and viscosity deviation ( Δη ) were calculated to reveal the variations in intermolecular interactions. Subsequently, the formation of intermolecular hydrogen bonds, primarily characterized by H 2 O···HNH- interactions, had been further confirmed through spectroscopic analyses, including Fourier-transform infrared (FTIR) and Raman spectroscopy. The CO 2 absorption performance of different mixed system was systematically investigated under varying gas flow rates and water concentrations. The results demonstrated that the mixed system with higher water content exhibited optimal CO 2 absorption capacity at elevated gas flow rates, reaching a maximum absorption of 1.11 mol CO 2 /mol AEEA. Cyclic absorption experiments were further conducted, and graphic characterizations, including Raman spectroscopy, infrared spectroscopy, and 13 C NMR, were utilized to analyze the CO 2 absorption process of the H 2 O + (PEG300 + AEEA) mixed system over time. It was found that the byproducts N-hydroxyethyl-2-imidazolidinone (HEIA) and 3-(2-hydroxyethyl)-2-oxazolidinone (HEOD), formed during the cycles, were the primary contributors to the decline in absorption capacity. As the number of cycles increased, the mixed system gradually reached a new chemical equilibrium, with absorption performance stabilizing. These findings offered valuable theoretical insight for the optimization of absorbent systems.
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