ACS Applied Energy Materials
·
2026
·
IF 5.5
Wu Pengxuan,Ding Yusong,Li Bingshuang,He Yunxia,Liu Qian,Huang Xiaoxi
This study reports a mesoporous carbon confinement strategy for enhancing the mass activity and structural durability of Au-based catalysts toward electrochemical CO 2 reduction reaction (CO 2 RR) to CO. Glutathione-protected Au clusters were introduced into polyaniline-derived mesoporous carbon (PDMC), followed by thermal ligand removal, producing ultrasmall Au nanoparticles uniformly embedded within a conductive N-doped carbon framework. The mesoporous carbon matrix effectively restricts Au growth and suppresses nanoparticle aggregation, thereby preserving abundant low-coordinated Au surface sites while maintaining accessible channels for charge and mass transport. The optimized Au@PDMC-30 catalyst delivers a CO Faradaic efficiency of 90.0 ± 1.3% at –0.9 V vs reversible hydrogen electrode in an H-type cell and maintains stable CO production for over 24 h without obvious Au aggregation. More importantly, under flow-cell conditions, Au@PDMC-30 achieves a high CO mass activity of 1192.4 mA mg –1 , approximately twice that of commercial Au/C, demonstrating greatly improved precious-metal utilization. In situ Fourier transform infrared spectroscopy and density functional theory calculations reveal that the confined low-coordinated Au sites possess an optimized electronic structure that facilitates *COOH formation, thereby accelerating the CO 2 to CO pathway. This work highlights confinement engineering of ultrasmall noble-metal nanoparticles as an effective route to improve catalytic selectivity, durability, and mass-normalized activity for CO 2 RR.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Dawei Zhang,Lei Huang,Haoyu Li,Menglin Niu,Zeeshan Abbasi,Yue Li,Tongqi Ye,Xuelan Hou,Maofeng Zhang,Jie Ren
The development of high-activity Ni-based catalysts for efficient CO2 methanation remains challenging, primarily due to Ni particle aggregation under high loading conditions, which limits their long-term stability at low temperature. To address this issue, this work evaluates the effect of doping with typical metals M (i.e., Co, La, Fe, and Ce) on the properties of Ni–Mg–Al layered double oxides (LDOs). The Ni–Co LDO (Ni/Co = 18:2, wt%), with the lowest activation energy (i.e., 54.5 kJ/mol), achieved 80% CO2 conversion and 99.9% CH4 selectivity at 350 °C, while Ni–La LDO only showed 73% CO2 conversion. The catalytic performance of optimized Ni–Co LDO is also quite stable under a 140 h time-on-stream thermal shock evaluation. Comprehensive characterization reveals that Co doping is particularly effective in generating abundant oxygen vacancies, creating numerous interfacial basic sites and stabilizing small Ni particles. In situ DRIFTS analysis further elucidates the resulting differences in reaction intermediates, pathways, and coordination environments, linking the enhanced structural properties to superior catalytic performance.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Bing-Bing Hong,Xue-Li Hu,Jing-Xuan Wang,Fu-Gen Chen,Yan-Yang Li,Jia Yang,Bei-Bei Zhang,Yi-Ke Li,Hong-Chang Yao,Zhong-Jun Li
Efficient photocatalytic conversion of CO2 into syngas is crucial for sustainable fuel production, yet conventional catalysts are often hampered by rapid charge recombination and insufficient surface area. Mesoporous single crystals (MSCs), which integrate a continuous single-crystal lattice with an open porous framework, offer a promising solution. Herein, we report a template-free strategy for synthesizing CdS MSCs in a NaOH–KOH–H2O eutectic medium, yielding materials with tunable mesopore sizes (2.9–4.2 nm) and high surface areas (111–185 m2·g–1). The optimized material achieves CO and H2 evolution rates of 7019 and 4027 μmol·g–1·h–1, corresponding to 38- and 12-fold increases over bulk CdS. Notably, the H2/CO ratio in the syngas product can be tuned by adjusting the cocatalyst dosage. The enhanced activity is attributed to the synergistic effects of large surface area, interconnected mesopores, and a continuous single-crystalline framework, which together facilitate charge separation and increase the density of accessible active sites. This work demonstrates a novel synthesis of mesoporous single-crystalline metal sulfides and establishes a generalizable strategy for designing high-performance photocatalysts. Its versatility is further evidenced by successful extension to NiO and Ni(OH)2, among other materials, suggesting potential applicability to a broader range of compounds.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Lin Li,Kunpeng Yu,Haixin Sun,Tong Feng,Dayu Liang,Qinqin Xu,Jianzhong Yin
Two-dimensional layered material membranes show great potential in the efficient sieving of molecules. However, balancing permeability and selectivity remains a significant challenge. In this study, ZIF-8 crystals are in situ grown on molybdenum disulfide (MoS 2 ) nanosheets exfoliated via supercritical carbon dioxide (scCO 2 ) for the first time, aiming to fabricate high-permeability MoS 2 @ZIF-8 membranes. It is suggested that the dispersed ZIF-8 crystals act as spacers to alleviate the restacking of MoS 2 nanosheets. The intrinsic microporous structure of ZIF-8, together with the tortuous transport pathways within the stacked MoS 2 layer, synergistically contributes to the size-selective separation performance of the membrane. Dye rejection tests show that the MoS 2 @ZIF-8 membrane exhibits high rejection rates and water permeability for various dye molecules. For example, the membrane has a rejection rate of 99.37% and a water permeability of 76.96 L m −2 h −1 ·bar −1 for Congo Red, and maintains an average rejection rate of 99.30% over 24 h of continuous operation. Moreover, the membrane can efficiently remove various dyes from salt-containing wastewater, with a maximum separation factor (SF) of 179.45 with a permeability of 79.77 L m −2 h −1 ·bar −1 . This method provides a promising solution for treating and purifying wastewater using membrane separation technology.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiapeng Ji,Zhibo Zhang,Zhixian Mao,Huajie Yin,Hui-Ming Cheng,Xiaolong Zhang
Novel Cu/CNTs-OH interface decouples gas/ion transport for acidic CO 2 conversion. • Interfacial H-bond network via -OH groups enhances proton mobility. • Shifts selectivity from ethylene to ethanol by optimizing *H coverage and proton supply. • In situ and theoretical evidences link H-bond network to key intermediates in ethanol pathway. Electrocatalytic CO 2 reduction (ECR) offers a route to convert CO 2 into valuable fuels such as ethanol, which is favored for its high energy density and ease of storage. ECR in acidic media could suppress carbonate formation but intensify competition from the hydrogen evolution reaction, limiting the selectivity of C 2+ products. Here we introduce an interfacial H-bond network strategy by coupling Cu nanoparticles with hydroxylated carbon nanotubes (CNTs-OH) to construct proton supply and steer reaction pathways for acidic CO 2 -to-ethanol electroconversion. Molecular dynamics and distribution of relaxation times analysis show that CNTs-OH enhance CO 2 diffusion while surface -OH groups form a dynamic H-bond network, facilitating proton transport via the Grotthuss mechanism. Density functional theory (DFT) calculations, isotope labeling, and rotating disk electrode results confirm that CNTs-OH promote water dissociation, supplying protons to Cu sites. In situ spectroscopy links the H-bond network to key ethanol pathway intermediates. Consequently, the introduced H-bond network at the electrode interface yields a 2.5-fold enhancement in ethanol selectivity and a dramatic shift in the ethanol/ethylene ratio from 0.4 to 1.6. This work provides an effective materials design strategy and mechanistic insight for selective CO 2 -to-ethanol conversion in acid media.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lin-Yuan Xiao,Chao-Yue Zhuo,Xiao-Nan Qin,Yue-Fei Zhang,Ziyi Li,Xiao Luo,Xiangjun Luo,Zhiwu Liang
Aminosilane concentration tunes Mg-MOF-74 structural evolution and porosity. • CO 2 adsorption exhibits high uptake at both ambient and high pressures. • The mechanism of how defects and amine groups synergistically enhance CO 2 capture capacity was studied. In this study, we report a rational design and synthesis of hierarchically porous 5/PA2-Mg-MOF-74@APTES with high CO 2 capacity through propionic acid (PA) modulation and amine functionalization (APTES). Characterization results confirmed that an optimized PA concentration effectively induced mesopore formation and exposed more unsaturated Mg 2+ sites, thereby generating hierarchical porosity, while subsequent grafting of APTES successfully introduced amino functional groups This combined strategy leverages both defect engineering and chemical functionalization, synergistically promoting CO 2 adsorption. Performance evaluations revealed that the optimal adsorbent 5/PA2-Mg-MOF-74@APTES(1:1), achieved a CO 2 uptake of 4.91 mmol·g −1 at atmospheric pressure (1 bar) and a remarkable uptake of 17.38 mmol·g −1 at high pressure (15 bar) with significantly improved CO 2 /CH 4 selectivity. This work explores a synergistic enhancement mechanism of CO 2 adsorption from the interplay of defect engineering and amine functionalization conducted by experimental characterization and theoretical calculations, which provides a novel strategy for the design and fabrication of high-efficiency CO 2 adsorbents suitable for diverse pressure applications.
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CHINESE JOURNAL OF CATALYSIS
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2026
·
IF 17.2
Haifeng Fan,Di Xu,Ting Zeng,Guoqiang Hou,Yangyang Li,Siyi Huang,Yanfei Xu,Zheng Wang,Xinhua Gao,Xiang-Kui Gu,Mingyue Ding
CO 2 methanation technology has shown great application prospects in carbon neutrality and hydrogen storage due to its extremely high energy efficiency and potential economic benefits. It is highly desirable but challenging to design novel catalyst and achieve efficient and stable CO 2 methanation under mild conditions. Herein, we developed a highly active electron-enriched Y 2 O 3 /Ni catalyst, achieving a stable operation with ~80.1% CO 2 conversion and ~100% CH 4 selectivity for 400 h at 0.1 MPa and 220 °C, which was a 100 °C lower than the conventional supported Ni-based catalysts. Structural characterizations confirmed that the Y 2 O 3 /Ni catalyst maintained dynamic redox changes and formed electron-enriched Y 2 O 3– x -Ni interfaces under reaction conditions. Mechanism studies proved that the Y 2 O 3– x -Ni interfaces obviously lowered the energy barrier of *HCO dissociation, and shifted the rate-determining step from *HCO dissociation to *CO hydrogenation. Furthermore, profited by the moderate CO x adsorption ability and higher H 2 coverage at the Y 2 O 3– x -Ni interfaces, the *CO hydrogenation reaction was kinetically promoted. The above factors accounted for the excellent low-temperature CO 2 methanation activity of the Y 2 O 3 /Ni catalyst.
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Chemical Science
·
2026
·
IF 8.1
Zhi-Hui Lv,Kang Liu,Chun-Qing Yin,Lin Du,Min Liu,Xin-Ming Hu
Direct electrochemical conversion of captured CO2 in amine solutions offers a promising route to upgrade dilute CO2 into valuable chemicals, bypassing the energy-intensive stripping step. However, this reaction is obscured by the complex equilibrium among carbamate, bicarbonate, dissolved CO2, and protonated ammonium in CO2-loaded amine solutions and suffers low selectivity due to the competing reduction of protonated ammonium. Here, we elucidate the reaction mechanism and reveal the mass transport as the governing factor for electrochemical conversion of captured CO2 in monoethanolamine (MEA), diethanolamine (DEA), and triethanolamine (TEA), which are the representatives of primary, secondary, and tertiary amines with the same functionality. Bicarbonate-derived CO2, rather than carbamate, is identified as the reactive species for CO generation across all amines. TEA is found to be the optimal amine, offering the highest CO selectivity (80%) and stability with heterogenized cobalt phthalocyanine as catalyst. This is attributed to the significantly hindered mass transport of both reactive bicarbonate and protonated ammonium in TEA than in the other two amines, with protonated TEA exhibiting particularly sluggish diffusion. These findings pave the way for the rational design of amine systems for efficiently converting captured CO2 through mass transport manipulation.
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CHEMICAL ENGINEERING & TECHNOLOGY
·
2026
·Vol. 49
·期 6
·e70256
·
IF 2
Yandi Li,Songyi Ji,Rong Zhang,Xiaoling Li,Xiandong Hao,Ning Zhao,Bo Wang,Zhiyong Xu,Wenbo Zhao
Carbon dioxide capture is critical for mitigating climate change. Amine-functionalized MIL-101(Cr) shows great promise due to its high stability and tunable porosity. We optimized its synthesis (160°C, 24 h, 150°C activation) and investigated diethylenetriamine (DETA) loading effects. The 50 wt% DETA composite achieved a CO 2 uptake of 1.25 mmol/g at 30°C and 0.1 bar, nearly six times that of pristine MIL-101(Cr). Kinetic and isotherm data were well described by the pseudo-second-order and Langmuir models. Thermodynamic analysis revealed Δ H = −54.78 kJ/mol and Δ S = −142.13 J/(mol K), confirming an exothermic, chemisorption-dominated process. We further optimized adsorption/desorption conditions, identifying optimal working temperatures of 269.47 K (adsorption) and 388.20 K (desorption). This work provides clear guidance for designing high-performance metal–organic framework (MOF)-based CO 2 capture materials.
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Nature Communications
·
2026
·
IF 18.1
Lei Jiwei,Wu Zihe,Ye Daoping,Feng Yifan,Tian Yu,Niu Jin,Liu Bowen,Wang Yi,Cheng Chong,Li Shuang,Zhao Changsheng
The catalytic conversion of CO 2 into value-added chemicals via the reverse water-gas shift (RWGS) reaction represents a significant pathway for mitigating climate change and enabling sustainable carbon utilization. However, Pt-based catalysts, despite their superior H 2 activation ability, often suffer from inadequate CO selectivity and durability under high-temperature conditions, primarily due to excessive CO adsorption at low-coordinated Pt edge sites. Herein, we present a sulfur (S)-mediated targeted passivation strategy to engineer Pt-CeO 2 catalysts with atomically tailored active sites, effectively addressing the critical activity-stability-selectivity trade-off. The incorporation of S into CeO 2 support induced optimized electronic modulation, as evidenced by in situ/ex situ characterizations and density functional theory (DFT) calculations, which weakened *CO adsorption strength and suppressed the methanation pathway. The optimized Pt-S-CeO 2 catalyst exhibits remarkable performance at 600 °C: CO selectivity >95%, CO production rate of 8.8×10 −5 mol g cat −1 s −1 , and <10% activity loss over 250 h. On the other hand, this work establishes a framework for targeted dopant-mediated site engineering in heterogeneous catalysis, offering a generalizable route to reconcile conflicting performance in CO 2 hydrogenation systems and beyond.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yinuo Wang,Yushen Liu,Ernest P. Delmo,Yian Wang,Zhehan Ying,Yan Zhang,Tiehuai Li,Xiaoyi Qiu,Ping Gao,Minhua Shao
An electrochemically-driven fluorine-erosion mechanism was proposed. • Active F species from GDL was generated during CO 2 RR through the mechanism. • Active F eroded the amorphous In hydroxides keeping high valence state for In. • In with high valance state facilitated CO 2 adsorption, promoting CO 2 RR. • High FE (93%) and partial current density (648 mA cm −2 ) of formate were achieved. Amorphous catalysts feature highly defective structures, providing more potential active site for electrochemical CO 2 reduction reaction (CO 2 RR). However, amorphous structures that lack control often lead to excessive side reactions and unforeseen structural reconstruction, largely suppressing the electroactivity. This study builds upon our earlier strategy relative to fluorine erosion, further elucidating an electrochemically-driven fluorine-erosion mechanism. Specifically, reactive fluorine species generated via the reversible electroreduction of polytetrafluoroethylene from the gas diffusion layer can effectively fluorinate amorphous indium hydroxides under CO 2 RR conditions, thereby creating active indium-fluorine content. This process enables the indium species to maintain a high valence state under electroreduction. Theoretical calculations demonstrate that fluorine-induced indium species facilitate CO 2 adsorption, promoting CO 2 RR pathway and subsequent formate production. The enhanced CO 2 RR performance can reach an impressive Faradaic efficiency of 93% at the partial current density of 648 mA cm −2 toward formate. This work sheds light on a novel approach for the structural control and modification for amorphous catalysts, highlighting a novel mechanism for fluorine erosion from the gas diffusion layer during electrocatalysis. Download: Download high-res image (244KB) Download: Download full-size image
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ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Haoran Han,Xuannuo Yi,Zhao Wang,Dan Chen,Aosheng Chang,Jinfeng Wang,Yaoyao Zhang,Wei Wang,Shasha Liu
With fossil fuels expected to remain a dominant global energy source, sustained CO2 emissions demand efficient mitigation strategies. Chemisorption-based postcombustion capture is widely applied due to its selectivity and operational simplicity. Understanding the absorption kinetics is critical for both elucidating fundamental reaction mechanisms and optimizing solvent performance. Herein, we present a prism-based reflection optical imaging platform integrated with a multichannel gas-injection system for quantitative, in situ, and high-throughput visualization of dynamic CO2 absorption in liquid absorbents. The approach exploited refractive index changes induced by CO2 absorption, detected as variations in reflected light intensity. The high-throughput capability enabled a direct comparison of absorption capacities and kinetic parameters within a single experiment. Monoethanolamine (MEA), diethanolamine (DEA), and N-methyldiethanolamine (MDEA) were investigated as representative primary, secondary, and tertiary alkanolamine absorbents. Kinetic analysis revealed that primary and secondary amines follow similar reaction pathways but exhibit different reaction rates, whereas tertiary amines proceed via a distinct mechanism and show a stronger dependence of the absorption rate on the absorbent concentration, characterized by distinct reaction orders and rate constants. This work established reflection-based optical imaging as a low-cost, versatile platform for high-throughput screening of gas–liquid absorption kinetics and for guiding data-driven absorbent discovery.
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