ACS Catalysis
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2026
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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
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2026
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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
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2026
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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
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2026
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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
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2026
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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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Science Advances
·
2026
·Vol. 12
·期 13
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IF 13.9
Decun Luo,Han-Xuan Liu,Zheng-Qing Huang,Xi-Yang Yu,Lei Chen,Riguang Zhang,Zhun Hu,Chun-Ran Chang
Frustrated Lewis pairs (FLPs) have emerged as a transformative strategy in small-molecule activation, leveraging steric inhibition to sustain highly reactive Lewis acid–base pairs capable of heterolyzing nonpolar molecules such as H 2 and CO 2 through electric field (EF)–induced polarization. Despite their promise, FLPs exhibit inherent limitations in activating highly stable, kinetically inert substrates, owing to insufficient field strength and limited polarization efficacy. The systems with intensified charge separation, termed frustrated ion pairs (FIPs), can transcend these constraints by combining extreme ionic reactivity with persistent frustration. Here, we propose a geometrically controlled FIPs system that systematically modulates interionic distance and interaction via cation size engineering, ensuring sustained frustration and remarkable catalytic enhancement. The relationship between the interaction strength of anions and cations in the FIPs and their performance in CO 2 cycloaddition exhibits a volcanic curve trend. FIPs catalysts with optimal distance (4.11 Å) and interaction strength (−78 kJ·mol −1 ·Å −1 ) between its cation and anion exhibit optimal catalytic performance ( TOF = 184 hour −1 ). The frustrated configuration liberates Br − from electrostatic confinement, achieving unprecedented nucleophilic activity by reducing the ring-opening energy barrier by 48.7 kJ·mol −1 compared to conventional ionic pairs. Optimal ion-pair distance in FIPs generates an intense asymmetric electric field that strongly polarizes CO 2 , yielding an induced dipole moment of ∆μ = 0.132 D. Moreover, the FIPs structure is extended to heterogeneous systems and exhibits a similar trend with homogeneous ones, showing its application potential.
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ENERGY & FUELS
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2026
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IF 6
Lei Yuan,Gang Zhu,Chenbao Lu,Qiqi Wan,Wenxing Jiang,Xiaodong Zhuang,Junliang Zhang,Changchun Ke
Membrane electrode assembly (MEA)-based CO2 electrolyzers are promising for industrial applications due to high energy efficiency and scalability, yet their long-term stability is severely limited by cathode salt precipitation. This work innovatively uncovers the salt precipitation mechanism from the perspective of water dynamics. This study clarifies that water plays dual key roles in regulating salt precipitation: first, as the essential carrier for cation removal, and second, as a dynamic modulator of transmembrane water and cation fluxes. Based on this insight, the concept of equivalent salt concentration (Ceq) is proposed, defined as the ratio of transmembrane potassium ion flux to liquid water flux. By comparing Ceq with the saturation solubility of KHCO3 (2.24 mol/L at 20 °C), a quantitative model is established to accurately predict the risk of salt precipitation under different anolyte concentrations, which is validated by long-term stability experiments. Systematic investigations show that membranes with high water permeability and low electro-osmotic drag (EOD) coefficients (e.g., X37–50 RT membrane reducing Ceq by 62.8% vs A40), enhanced gas diffusion layer (GDL) hydrophobicity, and optimized CO2 flow rates effectively mitigate salt precipitation. This work not only establishes a rapid prediction method for salt precipitation risk but also provides targeted strategies for the design of salt precipitation-resistant anion exchange membranes and GDLs in MEA CO2 electrolyzers, which is of great significance for advancing the industrial application of this technology.
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INORGANIC CHEMISTRY
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2026
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IF 4.6
Xiaoman Li,Yiming Wang,Xue Yang,Chaojin Jiang,Lulu Kong,Honghan Fei,Xueling Song
Organolead halide coordination polymers have emerged as promising photocatalysts owing to their attractive photophysical properties and structural tunability. However, organolead bromides typically exhibit limited photocatalytic performance due to their generally narrow light absorption range and inefficient carrier mobility. To overcome these issues, we designed and synthesized a robust layered organolead bromide coordination polymer templated by the squaric acid ligand featuring short carbon chains and broad near-UV absorption. It achieves visible light absorption and high charge separation efficiency, in contrast to the two reported lead bromide analogues with large interlayer spacing. Upon exposure to AM 1.5G simulated sunlight, the hybrid bromoplumbate exhibits enhanced photocatalytic activity for CO2–CO conversion, with high product selectivity and cycling stability. Moreover, the photocatalytic CO2 reduction performance is further promoted by in situ incorporation of trace Ag nanocrystals as reductive cocatalysts for suppressing carrier recombination, prolonging charge lifetime, and reducing free energy for the *COOH key intermediate. This work underscores the critical role of coordination chemistry in modulating the relationship between the structure and property of crystalline materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
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IF 3.9
Haixin Liu,Jintao Xu,Luming Qi,Zhenyang Rong,Jiaxuan Wang,Xiaoyang Tang,Zhaoyang Fei,Xian Chen,Qing Liu,Xu Qiao
The introduction of a porogen into a solid amine adsorbent was effective in enhancing the CO2 capture performance, structural stability, and long-term cycling stability. This study selected polyethylene glycol (PEG) as a porogen and prepared a series of CSP-nP-mT pellets, in which ZSM-5 served as the support, chitosan (CS) as the binder, and tetraethylenepentamine (TEPA) as the amine source. The results demonstrated that PEG effectively optimized the adsorbent pore structure, which enhanced the CO2 diffusion and improved accessibility to active amine sites. The structural optimization resulted in a significant increase in the CO2 adsorption capacity by 48.8% (from 1.74 to 2.59 mmol·g–1) compared to the sample without PEG. In addition to the improved adsorption performance, the compressive strength of CSP-1P-0.2T was 23% higher than that of CSP-0.2T. For the characterization of the adsorbent, N2 adsorption–desorption tests were employed to evaluate the pore structure of adsorbent pellets. SEM was used to measure the morphology of adsorbent pellets with different amounts of porogens. FT-IR and TGA were utilized to analyze the variation of functional groups and weight loss during the adsorption process. Furthermore, the adsorbents exhibited excellent cycling stability, retaining 87.2% of their initial capacity after 30 adsorption–desorption cycles. These results demonstrated that the incorporation of PEG in the adsorbent can effectively enhance the adsorption performance of solid amine adsorbents, which provided a strategy for developing high-performance adsorbents.
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CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 5.1
Yanmei Li,Chunjie Chen,Yali Zhao,Wufeng Wu,Yanying Wei,Haihui Wang
Two-dimensional metal–organic framework (MOF) membranes have emerged as competitive candidates for efficient gas separation owing to their ultrashort diffusion pathways and highly tunable nanochannels. However, unavoidable linker rotation within 2D frameworks constrain accurate molecular sieving. Herein, heteroleptic Zn(bim)(OAc) nanosheets are employed for constructing high-performance membranes, where cooperative 2D-3D linkers coupling regulates framework motions. The 3D acetate (OAc − ) linkers limit the amplitude of motion, whereas planar 2D benzimidazolate (bim) linkers introduce locally rotational freedom through weaker M−N coordination bond, generating precise angstrom-level, dynamically tunable pore window. The heteroleptic membrane achieves considerable H 2 /CO 2 selectivity of ∼ 134, surpassing the upper bounds of traditional polymer membranes. This work demonstrates that cooperative 2D-3D linkers coupling provides a feasible pathway to engineer precise, dynamically tunable apertures in 2D MOF nanosheet membranes, offering a promising avenue for designing high-performance membranes.
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Green Energy & Environment
·
2026
·
IF 16.7
Guohua Li,Xiaodi L,Wei Zhang,Di Cai,Hui Cao,Zehan Yao,Tõnu Pullerits,Kaibo Zheng,Tianwei Tan
Photochemical regeneration of NADH is essential for bioinspired redox catalysis but remains limited by inefficient electron-proton coordination. We report a donor-acceptor conjugated polymer system with rhodium centers, where electron-donating substituents (-OH, -OMe, -Me) can modulate both photo-induced charge behavior and surface reaction properties. The optimal -OH subsitutents can, on one hand, enhances dielectric screening and planarity of the polymers to, reduce the exciton binding energy and facilitate charge injection to the rhodium active centers. On the other hand, its hydrophilicity further promotes proton migration, enabling synchronized and co-localized two-electron/one-proton donation to NAD + at the rhodium centers. Therefore, the optimized -OH-containing polymer achieved selective photoreduction of NAD + to 1,4-NADH at a rate of 12.81 mmol g -1 h -1 , which is one of the highest levels reported to date to our knowledge. Integrated into a photo-electro-enzyme cascade, the system synergistically couples NADH regeneration with enzymatic catalysis to achieve the first conversion of CO 2 -derived aldehydes into glycerol, highlighting its potential for sustainable carbon valorization. This work establishes a facile strategy to regulate both electron and proton donation in organic photocatalysts and expands their application in solar-driven biotransformations.
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