MOLECULES
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2025
·Vol. 30
·期 12
·2573
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IF 4.6
Jinliang Lin,Rongying Liao,Li Li,Shuli Yao,Shengkai Li,Yun Zheng,Fei Fei
Photocatalytic CO2conversion is one of the ideal approaches to address both topics of solar energy shortage and carbon neutrality. Cobalt(II) centers coordinated with bipyridines have been designed and evaluated as catalysts for CO2conversion under light irradiation. Herein, we report a series of pyridine-based cobalt complexes with alkyl substituents as molecular photocatalysts, aiming to elucidate the effects of alkyl type and substitution position on catalytic performance through spectroscopic and electrochemical measurements. The substitution of the hydrogen at 4,4′-positions on the bipyridine ring with a methyl group, a tert-butyl group, and a nonyl group led to a decrease in the conversion rate of CO2by 13.2%, 29.6%, and 98%, respectively. The methyl substituents at the 5, 5′-positions of the bipyridine ring resulted in a 71.1% decrease in the CO2conversion rate. The usage of either 6, 6′-Me2-2,2′-bipy, 2,4-bipy, or 3,3′-bipy resulted in no detectable activity for CO2conversion in the current system. Both photo- and electrochemical analyses have been employed to reveal the relationship between changing ligands and photocatalytic performance on the molecular scale. These results demonstrate that bulky ligands significantly hinder CO2reduction by cobalt complexes due to steric interference with coordination and active-site accessibility. This study demonstrates that the substituent effect of ligands on photocatalytic reactions for CO2conversion provides valuable insight into a deeper understanding of molecular catalysis.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Chenhui Qiu,Lei Wang,Ruijie Chen,Gongde Wu,Jie Zhang,Jing Ding,Jun Li,Jinfeng Zhang,Hui Wan,Guofeng Guan
Synthesizing value-added solar fuels represents a promising solution to address energy and environmental issues. Its efficiency is determined by the performance of photocatalysts, and the main challenges lie in achieving efficient interfacial charge transfer and utilization, which are highly related to the assembly of cocatalysts. Herein, we design La 3+ -defect LaFeO 3 nanofibers with a higher specific surface area to achieve highly dispersed loading of Ag nanoparticles through a one-step coaxial electrospinning technique. Characterizations and theoretical calculations revealed that La 3+ defects favor the anchoring of Ag nanoparticles and the formation of a Schottky junction, thereby facilitating the interfacial charge separation and transfer. Additionally, this synergistic engineering efficiently boosts CO 2 adsorption/activation and strengthens the proton affinity, preferentially driving the multi-electron reduction. Owing to these benefits, the optimized nanofibrous Ag/La 0.9 FeO 3 sample exhibits promising photothermal catalytic performance, yielding CH 3 OH of 7.12 μmol·g -1 ·h -1 , which is 2.8-fold over pristine LaFeO 3 , along with good stability and selectivity. This work highlights the effect of interfacial construction on developing advanced photocatalysts.
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POLYMER
·
2025
·
IF 4.5
Wensi Li,Jiajia Ye,Jingjing Liu,Yufei Song,Juan An,Zhen Kong,Jibin Song
A novel porous fluorescent material based on polyhedral oligomeric silsesquioxane (POSS) functionalized with imidazole-selenone has been synthesized using a one-pot Povarov reaction. Comprehensive characterization reveals that the product of Polyhedral oligomeric silsesquioxane-Se1-triphenylamine which denoted as POSS-Se1-TPA exhibited exceptional thermal stability, fluorescence properties, and thermal stability, making it highly suitable for detection of heavy metal ions and CO 2 adsorption. The incorporation of imidazole selenone, quinoline structures, and triphenylamine groups has enabled POSS-Se1-TPA with multi-site binding, facilitating high sensitivity and selectivity towards Fe 3+ and Cu 2+ ions. Furthermore, CO 2 adsorption studies have revealed its capacity of 28 mmol/g at 700 mmHg, attributed to microporous structures and active functional groups that promote physisorption and chemisorption mechanisms. POSS-Se1-TPA, as a dual-function material has provided an innovative platform for environmental monitoring, including efficient metal ion detection and gas adsorption, and served as a model for designing advanced functional materials with versatile applications in sensing, bioimaging, and environmental remediation.
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ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Tianlong Tan,Hai Liu,Wenlong Cao,Lei Yang,Shujing Ju,Caiyu Chen,Ewald Janssens,Guowei Han,Dachun Lu,Jue Wang,Qinfang Zhang
The electrochemical CO2 reduction reaction (CO2RR) is one of the most promising pathways to achieving carbon neutrality. However, in acidic electrolytes, the CO2RR tends to suffer from competitive hydrogen evolution side reactions. Alkaline electrolytes are typically employed to suppress side reactions and promote the formation of valuable multicarbon (C2+) products (e.g., ethylene(C2H4)). In this study, we fabricated surface-loaded copper cluster catalysts with particle sizes below 5 nm by magnetron sputtering and inert gas condensation in combination with cluster beam deposition. This approach enabled precise control over the catalyst surface structure, allowing for in-depth investigation of the synergistic effects between the catalyst microstructure and its catalytic microenvironment. We demonstrate that the Faradaic efficiency (FE) for CO2-to-C2H4 conversion exceeds 50% across a broad current density range of 50 to 180 mA cm–2 in a flow cell using 1 M KOH electrolyte. Compared with a pristine Cu/PTFE catalyst, the optimized Cu cluster catalyst not only exhibits a significant enhancement in FEC2H4 but also expands the effective current density range. Furthermore, finite element simulations combined with in situ Raman spectroscopy reveal synergistic interactions among interfacial species (e.g., *CO, OH–, and K+). Therefore, this study proposes a general strategy to regulate the dynamic evolution of catalytic interfaces through an initial nanostructure design, thereby opening a promising avenue for the selective conversion of CO2 to ethylene.
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ACS Omega
·
2026
·
IF 5.2
Malesela A. Mafokoane,Peixi Liu,Xiaoxia Ou,Nicholas M. Musyoka,Fei Chang
The reduction of carbon dioxide (CO2) to methanol (CH3OH), is presently constrained by energy-intensive processes requiring high temperatures and pressures to overcome kinetic and thermodynamic limitations. This work unveils for the first time a reaction pathway for alkali and alkaline earth metal hydrides (LiH, NaH, KH, MgH2, CaH2, and BaH2), enabling the activation and selective reduction of CO2 to methanol under ambient pressure. This finding represents a significant departure from the established paradigm, which exclusively produced methane at moderate pressures (0.1–1 MPa). Temperature-programmed reaction studies reveal that these metal hydrides function synergistically as both hydrogen sources and promoters for CO2 reduction, exhibiting hydrocarbon production within specific temperature windows. Systematic screening identifies lithium hydride (LiH) as the most effective material, with a maximum production rate of 0.182 μmolMeOH·molmetal–1·h–1 at 245 °C under ambient pressure, highlighting a structure–activity relationship governed by metal-formate stability. Through mechanistic investigation, we elucidate a formate (HCOO*)-mediated pathway wherein the hydride ion serves as a potent nucleophile, directly reducing CO2 without the need for high H2 partial pressures. This discovery provides a transformative framework for the sustainable synthesis of CH3OH and lays the groundwork for the development of next-generation materials incorporating reactive ionic hydrides for the conversion of CO2 under mild conditions.
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ENERGY & FUELS
·
2026
·
IF 5.3
Jian Wen,Yangfeng Zheng,Cheng Zhai,Hexiang Xu,Yu Wang,Hongda Wen,Zijian Yu,Huijun Xing
Injecting CO2 foam fracturing fluid into coal seams leads to modifications in the coal’s pore structure, which directly affects coalbed methane (CBM) recovery. Among the influencing factors, the duration for which the CO2 foam remains within the coal seam plays a critical role. This study examines how the pore structure of Zhangminggou bituminous coal evolves after treatment with a CO2 foam fracturing fluid for different durations. Experiments were conducted at 40 °C and 5 MPa, with treatment durations of 3, 6, 12, 24, and 48 h. The evolution of the pore structure in modified coal was analyzed through nuclear magnetic resonance and low-temperature nitrogen adsorption techniques. Results show that pore structure evolution is strongly time-dependent. Relative to untreated coal, foam-treated coal exhibits an increase in micropores but a decrease in average pore size, alongside a moderate rise in mesopores and a marked increase in macropores and fractures. Fractal analysis of NMR images indicates that the opening size of the generalized fractal dimension spectrum and the width of the multifractal singularity spectrum both increase with treatment time, which reflects growing spatial complexity and heterogeneity in pore distribution. Low-temperature nitrogen adsorption results reveal that the specific surface area, total pore volume, and average pore diameter increase with treatment time, following a power-law relationship. The pore volume distribution shifts from 2–10 nm toward >50 nm, with a rising proportion of pores larger than 50 nm. These findings provide valuable insights for optimizing the CO2 foam fracturing parameters in practical applications and enhancing CBM recovery.
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ACS Catalysis
·
2026
·
IF 13.1
Wendong Wang,Xingwen Cha,Longmei Shang,Kang Sun,Fangsong Guo,Jianchun Jiang,Guowu Zhan
This work demonstrates a strategic shift from dynamic electrolyte modulation to static, intrinsic promotion of the CO2 reduction reaction by stably integrating alkali metal cations as a solid-state component within a heterogeneous catalyst. To address the persistent challenge of alkali metal ion leaching due to high aqueous solubility, we immobilize K+ cations into a carbon nitride framework (Ni@K–C3N4) hosting atomically dispersed Ni–N3 sites via an ionothermal strategy. Structural confinement through coordination with nitrogen sites in the C3N4 matrix effectively suppresses K+ leaching, enabling sustained electronic regulation of the Ni centers. Combined experimental and theoretical analyses reveal that K+ incorporation attenuates d-π conjugation, promotes electron localization around Ni sites, and stabilizes low-valent Niδ+ species. This electronic reconfiguration enhances CO2 adsorption and activation while suppressing competitive hydrogen evolution reaction. The optimized Ni@K–C3N4 catalyst achieves a CO Faradaic efficiency of 95% at −0.74 V vs RHE, a current density of ∼20 mA·cm–2, and stable operation over 50 h. Notably, it maintains >80% CO selectivity under a diluted CO2 atmosphere (40%), highlighting its practicality for real low-concentration streams. This work establishes a polymer-functionalization strategy for precise electronic tuning of single-atom catalysis, advancing the design of efficient CO2 utilization systems.
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ACS Catalysis
·
2026
·
IF 13.6
Shuangfeng Ren,Yihui Li,Ye Chen,Xiaoling Mou,Ziang Zhao,Hejun Zhu,Xiaoyan Liu,Yu Meng,Li Yan,Apoorva Ravi,Amol Amrute,Ronghe Lin,Yunjie Ding
The rational design of selective, earth-abundant Ni-based catalysts for the reverse water–gas shift (RWGS) reaction is often hampered by an incomplete understanding of their operando active states. This study reveals that the CO2 hydrogenation selectivity over Ni–Zn catalysts is governed by a support-dependent, reaction-induced dynamic restructuring, rather than by any static, preformed sites. Through a combination of in situ characterization and theoretical calculations, we demonstrate that the active Ni–Zn intermetallic core encapsulated by ZnO forms dynamically only under the RWGS atmosphere on ZrO2 and TiO2 supports, but not on Al2O3 or during mere H2 reduction. Crucially, we identify in situ-generated CO as the essential inducer of this reconstruction, likely via facilitating ZnO reduction. Furthermore, the product selectivity (CO vs CH4) is dictated by the kinetic competition between CO desorption and its deep hydrogenation, a principle quantitatively linked to the evolved electronic structure of the active surface. This work shifts the paradigm toward designing catalysts that evolve into optimal structures in operando and provides a fundamental kinetic framework for selective CO2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Ziyan Yang,Chunqi Yang,Yihua Zhu,Ling Zhang,Yuhang Li,Chunzhong Li
The Bi O bond is widely regarded as the key motif for CO 2 electroreduction towards formate, but the role of specific Bi O coordination remains unclear. Herein, we study the electrocatalytic behavior of a Bi 4 Ti 3 O 12 perovskite containing Bi O 6 and Bi O 7 structures. Under 24-h CO 2 reduction reaction (CO 2 RR), Bi 4 Ti 3 O 12 reconstructs into Bi 2 O 2 CO 3 while retaining Bi O 7 and maintaining high formate Faradaic efficiency (FE). In contrast, electrochemical measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirm Bi 2 O 3 lacking Bi O 7 favors hydrogen evolution reaction (HER). Density functional theory (DFT) calculations indicate Bi O 7 lowers the energy barrier for *OCHO generation, identifying it as the key active site. Using a solid-state electrolyte (SSE) reactor, pure formic acid (0.19 M) is continuously produced with ∼70% FE over 48 h. This work indicates that the coordination environment of Bi O motif displays an essential role in selectivity, and that the Bi O 7 motif might be the critical active site for formate production.
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Polymer Chemistry
·
2026
·
IF 3.9
Mengchao Zhang,Sifan Li,Zhaohui Zhang,Hongkun Li
The direct conversion of carbon dioxide (CO2) into value-added polymeric materials has garnered considerable research interest in recent decades. Multicomponent tandem polymerization (MCTP), as an emerging synthetic strategy, demonstrates exceptional efficiency in constructing functional polymers. Nevertheless, CO2-involved MCTP systems have been rarely reported. Herein, we developed a one-pot MCTP involving CO2, alkynes, alkyl bromide, and thiol, enabling the efficient transformation of CO2 into structurally well-defined regioregular polymers. The polymerization process mediated by Ag2WO4 and Cs2CO3 under ambient pressure in N,N-dimethylacetamide upon heating produced four soluble poly(β-thioacrylate)s with high weight-average molecular weights (up to 11 500 g mol−1) and Z-stereoregularities (up to 84%). Notably, the tetraphenylethene-containing polymer exhibited aggregation-induced emission features, demonstrating its potential as a dopant in liquid crystalline polymer networks. The resulting film displayed circularly polarized luminescence properties with an exceptional luminescence dissymmetry factor of −0.88. Intriguingly, the polymer/polyamide 6 (PA6) composites manifested room-temperature phosphorescence featuring long emission lifetimes up to 510 ms. Furthermore, the polymers could be post-modified by the thiol–ene click reaction to produce sulfur-rich polymers. This work provides a robust platform for converting CO2 into stereoregular polymeric materials with tailorable photophysical properties, offering promising applications in advanced optoelectronic materials and sustainable technologies.
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GREEN CHEMISTRY
·
2026
·
IF 10.6
Qizhou Xue,Jiaqi Feng,Boyang Liu,Yanlin Wang,Aofei Cheng,Chongyang Jiang,Xiaofu Sun,Min Wang,Yinge Bai,Shaojuan Zeng,Xiangping Zhang
Non-metal element doping has emerged as an effective strategy to modulate electrochemical CO2 reduction reaction performance. However, current research predominantly focuses on individual doping configuration (interstitial doping or substitutional doping), and systematic investigations into the effects of different doping types on electrocatalytic activity remain scarce. This limitation significantly hinders the rational design and broader implementation of doping strategies. In this work, we successfully prepared two distinct selenium (Se)-doped bismuth catalysts (interstitial doping and substitutional doping) and systematically investigated the effects of these two doping configurations on the performance of CO2 electroreduction to formate. Detailed experimental and theoretical studies revealed that Se interstitial doping facilitated more efficient electron transfer to the active Bi sites compared to substitutional doping, thereby enhancing the stability of key intermediate *OCHO and lowering the free energy barrier for its formation. Meanwhile, Se interstitial doping more effectively suppressesd the hydrogen evolution reaction. As a result, Se interstitial doping Bi displayed > 90% formate Faradaic efficiency (FE) at an ampere-level current density (0.9 A cm-2 – 1.3 A cm-2) in pH-universal (acidic, pH=1.2; neutral, pH=7; and alkaline, pH=14) electrolytes and a maximum formate FE of 98.1% was achieved in alkaline electrolyte. This work provides new insights into the structure-function relationship of Se doping configurations and offers a rational design strategy for developing highly selective and efficient catalysts for CO2 electroreduction.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Miao Miao,Qijie Jin,Yan Shao,Feng Zeng,Huanhao Chen
This study developed a ternary CuCoIn/Al 2 O 3 catalyst for the direct hydrogenation of CO 2 to ethanol. The incorporation of Co and In species created a synergistic effect that enhanced CO 2 interaction and activation. This synergy also modulated the electronic state of surface Cu atoms, increasing the proportion of Cu + species, which promoted the non-dissociative adsorption of CO and the formation of *HCOO intermediates. These changes significantly enhanced C C coupling, leading to the generation of key ethoxy intermediates. The optimized catalyst, with a Co/(Co + Cu) ratio of 0.08 and 1.5 wt% In loading, achieved over 90% ethanol selectivity among total alcohols at 260 °C, along with a relatively high ethanol production rate of 33.0 g EtOH kg cat −1 h −1 . This work presented an effective strategy for designing high-performance, non-precious metal catalysts for selective CO 2 -to-ethanol conversion.
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