JOURNAL OF THE ENERGY INSTITUTE
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2026
·
IF 6.5
Haifei Wang,Wei Tian,Yunlong Tian,Zhiqiang Han,Chengzhuang Zhang,Kun Liang,Gebrehiwot Gebreslassie,Denggui Wang,Jia Fang
Nitrogen-doped biochars are prepared from corn stalk using different potassium salts (KOH, KHCO 3 , K 2 CO 3 , and potassium citrate) as activators, followed by KCl-assisted modification. Among all samples, PB2 (K 2 CO 3 /KCl co-activated) shows the highest CO 2 uptake of 4.28 mmol/g at 25 °C and 1 bar. This improved performance is attributed to the combined effects of abundant ultramicropores and narrow micropores, particularly pores below 0.6 nm, together with abundant surface functional groups, including graphitic nitrogen and C-N/C-O species. The micropores provide a high density of adsorption sites, which promotes efficient pore filling. Meanwhile, the nitrogen and oxygen functionalities enhance CO 2 affinity by modulating the electronic properties and increasing surface polarity. Cyclic stability is evaluated by thermogravimetric analysis (40 °C, atmospheric pressure). PB2 exhibits an initial CO 2 adsorption capacity of 2.05 mmol/g, which decreases to 1.69 mmol/g after five adsorption-desorption cycles, corresponding to a capacity retention of 82.44%. Although this cyclic performance is lower than those of PB, PB1, and PB3, PB2 combines the highest single-point CO 2 uptake with acceptable cyclic stability. This result indicates a trade-off between adsorption capacity and cycling stability. Overall, the results demonstrate that both pore structure and surface chemistry are critical to CO 2 adsorption performance. Among all samples, PB2 exhibits the most favorable combination of these characteristics.
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Nano Energy
·
2026
·
IF 16.7
Maoxiang Li,Yachao Xu,Shijie Liu,Zihan Ma,Zhaojun Sun,Jianwei Zhang,Ying Wang,Mingyi Zhang
A strained Pd-O-Ti interface with abundant oxygen vacancies forms an electronic potential-well CO-hydrogenation box. • Spatial coupling of CO confinement and hydrogen activation enables exclusive CO 2 -to-CH 4 photoreduction. • This interfacial design provides a general strategy for deep CO 2 hydrogenation products. Solar-driven conversion of CO 2 to methane offers a route to carbon-neutral fuels, but directing the multielectron pathway beyond the CO intermediate remains a central challenge. Here, by growing Pd nanoparticles in situ on oxygen-deficient TiO 2 (Pd/TiO 2-x ), we construct an oxygen-vacancy-rich Pd-O-Ti interface that functions as a CO-hydrogenation box. Interfacial oxygen vacancies enrich and retain CO 2 -derived carbon intermediates, whereas adjacent Pd sites promote H 2 O activation and provide reactive surface hydrogen species in the same nanoscale region. This spatial coupling of CO confinement and hydrogen delivery favors sequential C-H bond formation and suppresses premature CO desorption, thereby redirecting CO 2 photoreduction toward CH 4 . As a result, Pd/TiO 2-x achieves 100% CH 4 selectivity with a CH 4 production rate 40 times higher than that of TiO 2 under AM 1.5 G irradiation. Under natural sunlight, the catalyst delivers a CH 4 production rate of 1.1 mmol h −1 g −1 and sustained activity over repeated daytime cycles. These results identify an interfacial design principle for steering multielectron CO 2 photoreduction toward deeply reduced hydrocarbon products. Download: Download high-res image (199KB) Download: Download full-size image
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JOURNAL OF CATALYSIS
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2026
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IF 6
Mufan Niu,Qiyu Sun,Chongbin Wei,Fubin Peng,Xiaohe Huang,Han Yang,Ying Cui,Shenyong Ren,Chunming Xu,Baojian Shen
To elucidate the active sites and reaction mechanism of CrO x /ZrO 2 catalysts in CO 2 -assisted oxidative dehydrogenation (CO 2 -ODH) of ethane, a combination of multiple characterization techniques, DFT calculations, and in situ FTIR spectroscopy was employed. Results reveal the coexistence of isolated and polymeric Cr 6+ species on the catalyst surface, with catalytic activity exhibiting a strong positive correlation with the content of polymeric Cr 6+ , confirming its role as the key active component. Further investigation uncovers a distinct and strong electronic interaction between CrO x and ZrO 2 that facilitates the formation and stabilization of polymeric Cr 6+ . This interaction is absent in CrO x /CeO 2 and CrO x /TiO 2 systems, offering a theoretical rationale for the rational design of catalyst supports. Mechanistically, CO 2 plays a dual role: it participates in both ethane ODH and the RWGS reaction, and reoxidizes coordinatively unsaturated Cr 3+ to Cr 6+ , thereby enhancing reaction stability. This work elucidates the CO 2 -ODH pathway and the regulatory role of CO 2 , offering new insights into the design of active sites in CrO x -based catalysts. However, pronounced catalyst deactivation currently limits industrial application, highlighting the need for future efforts to focus on improving catalyst stability.
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Solar RRL
·
2026
·Vol. 10
·期 2
·e202500917
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IF 4.7
Lu Peng,Qiang Li,Siting Shao,Meng Zhang,Hongpeng Jia
The escalating CO 2 concentration and energy demand necessitate efficient CO 2 conversion strategies. Photothermal catalytic CO 2 methanation is a promising strategy, yet its efficiency is hindered by the inherent stability of CO 2 and the rapid recombination of photogenerated charge carriers. Among non-noble metal catalysts, Ni-based catalyst is a promising candidate for CO 2 methanation, with sintering and agglomeration remaining to be addressed. Herein, NiMn/TiO 2 bimetallic catalysts with varying Ni/Mn ratios were synthesized to overcome these issues. Characterization results demonstrate that Mn incorporation enhances CO 2 adsorption capacity by increasing oxygen vacancies and significantly improves the separation efficiency of photogenerated carriers. Furthermore, Mn doping optimizes the electronic structure of the catalyst, narrowing its bandgap for improved light absorption. But the catalytic performance is highly dependent on the Ni/Mn ratio. The synergistic effect of Ni and Mn can be maximized when the Ni/Mn ratio is 1:1, which is specifically manifested as the best catalytic activity. Excessive Mn loading covers active Ni sites and impedes electron transfer, thereby degrading activity. Therefore, this work highlights the importance of Mn as a promoter in designing efficient non-noble metal catalysts for photothermal CO 2 conversion.
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Small
·
2026
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IF 12.1
Yu Liu,Yi Xin,Teng Zhang,Yunlong Li,Junhong Jian,Shoufu Cao,Jian Luan,Xiaosa Zhang,Wenze Li,Wei Qi
Tailoring bimetallic synergy in azo-functionalized porous organic polymers for enhanced electrocatalytic CO 2 reduction porous organic polymers (POPs) have emerged as promising candidates for electrocatalytic applications due to their structural tunability and high surface areas. In this study, we report a coordination-driven assembly strategy to construct a Cu/Co bimetallic azo-phenolic polymer (denoted as Cu@Azo-CoPG) through chelation of azo-phenolic motifs with Cu 2 + ions. Systematic evaluation reveals that the bimetallic Cu@Azo-CoPG outperforms its monometallic counterparts (Cu-PG and Co-PG) in CO 2 reduction reaction (CO 2 RR), achieving a remarkable CO Faraday efficiency (FE CO ) of 94.3%. First-principles calculations elucidate that the Cu─Co dual sites synergistically modulate reaction energetics: the Co center lowers the energy barrier for * COOH intermediate formation, while adjacent Cu sites facilitate CO desorption. This work establishes a design paradigm where the electronic interplay between heterometallic sites in POPs enhances both CO 2 adsorption/activation and product desorption kinetics, offering new insights into the rational engineering of dual-active-site catalysts for sustainable energy conversion.
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ADVANCED MATERIALS
·
2026
·
IF 26.8
Kangwang Wang,Jie Zhan,Jun Liu,Zaichen Xiang,Wanyi Zhang,Lingyong Zeng,Kai Yan,Yan Sun,Huixia Luo
The photochemical CO 2 reduction reaction (CRR) represents a zero-carbon pathway for converting CO 2 into value-added chemicals, yet its industrial implementation has been constrained by low selectivity and product diversity. Dirac nodal arc semimetals characterized by ultrahigh carrier mobility (>25 000 cm 2 ·V −1 ·s −1 ) offer a promising platform to search for efficient catalysts for CO 2 conversion. Herein, we demonstrate that strategic Pt incorporation into PdSn 4 optimizes the electronic structure and carrier dynamics of this Dirac semimetal. Experimental and theoretical analyses reveal that the resulting Pd─Sn─Pt local electronic structure redistributes charge density around Pd and Pt atoms, which facilitates C─C coupling via *OC─COH and *OC─CHOH intermediates and enhances carrier mobility by 40% versus the pristine PdSn 4 single crystal. The optimized Pd 0.4 Pt 0.6 Sn 4 single crystal achieves C 2 H 4 i) formation rate of 328 µmol∙g −1 ∙h −1 ; ii) product selectivity of 73.1%; iii) electron-based selectivity of 89%. This work establishes electronic-structure-tunable Dirac semimetals as a new paradigm for multi-carbon photochemical CO 2 reduction, providing a design strategy for next-generation photocatalysts.
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AICHE JOURNAL
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2026
·
IF 4
Ningbo Yu,Shaofei Wang,Min Zhou,Min Xiao,Bo Jin,Hongxia Gao,Zhiwu Liang
Amine-based water-lean solvents serve as energy-efficient absorbents for carbon dioxide (CO 2 ) capture but face paradoxical kinetic challenges, where the mixed solvents inconsistently accelerate or decelerate reaction rates across amine classes. By integrating stopped-flow kinetics, molecular dynamics simulations, and electrostatic potential analysis, we elucidate water modulates CO 2 absorption in mixed absorbents systems via amine-specific solvent encapsulation effect for the first time. For primary amines (e.g., monoethanolamine, MEA), water preferentially hydrates nucleophilic nitrogen atoms, forming steric barriers that impede CO 2 access and suppress kinetics with increasing hydration. Conversely, secondary amines (e.g., methylaminoethanol, MAE) exhibit oxygen-directed hydration, which weakens nitrogen solvation and enhances electrostatic CO 2 -amine interactions, accelerating kinetics. A zwitterion-based kinetic model quantifies these solvent-induced activation energy shifts, revealing a universal mechanism validated across diverse solvent systems. This work establishes molecular design principles for tailoring water-lean absorbents, bridging the critical gap between solvent engineering and reaction pathways to advance energy-efficient carbon capture technologies.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Yongjun Mao,Yudian Zhu,Xudong Wang,Jianming Liu,An-Ping Zeng
The synthesis of amino acids from CO2 as the sole carbon source is a critical goal for sustainable biomanufacturing, offering a green alternative to conventional production methods plagued by greenhouse gas emissions and resource competition. Here, we construct a highly efficient cell-free enzymatic platform for the direct biosynthesis of aspartate from CO2. Our integrated platform couples a carbon-fixing module using the modified reductive glycine pathway (rGlyP) with a custom-designed synthesis cascade that condenses two glycine molecules into aspartate, driven by glycine oxidase and a redesigned b-hydroxyaspartate cycle (BHAC). A key challenge in this multienzyme system is achieving pathway synergy. To address this, we employed an enzyme-constrained static model to rationally design the optimal stoichiometry of the five-enzyme cascade. This computational approach not only boosted the final aspartate yield by over 25% but was also essential in identifying glycine oxidase (Bs-ThiO) as the primary rate-limiting bottleneck. Through systematic optimization of enzymes, reaction conditions, and feeding strategies, the system finally achieved accumulation of 17.3 mM aspartate (2.3 g/L) within 2 h, reaching an exceptional 92% of the model-predicted theoretical yield. This study establishes a powerful and sustainable platform for green amino acid production and showcases the significant potential of combining computational design with cell-free engineering to advance the frontier of CO2-based biomanufacturing.
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ACS Catalysis
·
2026
·
IF 13.6
Xianglong Meng,Yanjiao Wang,Ruiping Deng,Soryong Chae,Chunzheng Wang,Girolamo Giordano,Zifeng Yan,Hailing Guo,Svetlana Mintova
A strategy for synthesizing bimetallic catalysts confined within zeolite frameworks, offering a promising approach for stabilizing metal species under harsh reaction conditions, is disclosed. A dual-stage synthesis strategy including alkali etching to open the channels of Silicalite-1 (S-1) zeolite, exposing internal hydroxyl defects that serve as anchoring sites for Cu and Zn species, is presented. This was followed by a dry-gel conversion encapsulation step to yield Cu-ZnO@S-1 catalyst. The competitive occupation of these sites by Cu and Zn facilitates the formation of high-density Cu-ZnO interfaces. Under reaction conditions of 3 MPa and 250 °C, the catalyst achieves a methanol selectivity above 99.2% and a space-time yield (STY) of 2.1 g gCu–1 h–1, nearly four times higher than that of copper-containing catalyst (Cu@S-1, 0.54 g gCu–1 h–1) and significantly outperforming the sample prepared by conventional impregnation (Cu-ZnO/S-1, 1.6 g gCu–1 h–1). The oxygen-deficient Cu-ZnO1–x sites at the Cu-ZnO interface are further demonstrated to serve as genuine active centers for methanol synthesis. The methanol formation reaction proceeds via the formate pathway, and the high density of Cu-ZnO1–x sites effectively lowers the activation barrier for the hydrogenation of *HCOO to *H2COO.
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ACS Applied Energy Materials
·
2026
·
IF 5.5
Tongxin Qu,Yongchun Zhao,Zhuo Xiong,Junying Zhang
Electrocatalytic CO2 reduction reaction (eCO2RR) offers a sustainable route for converting CO2 into value-added chemicals, contributing to carbon neutrality. While high selectivity toward C1 products has been achieved, the efficient production of multicarbon (C2+) compounds remains challenging due to the high energy barriers of C–C coupling. Copper-based catalysts are promising for C2+ generation owing to their unique *CO binding energy, yet they suffer from low selectivity and stability. Alloying copper (Cu) with other metals is an effective strategy for regulating intermediate adsorption and facilitating C–C coupling. In this study, an efficient CuGa solid solution alloy electrocatalyst for the eCO2RR was synthesized, employing only straightforward immersion drying and subsequent reduction annealing processes. At an applied potential of −1.19 V vs RHE, this catalyst exhibited a high Faradaic efficiency of 66.27% for C2+ products, significantly suppressing C1 pathways. It also demonstrated remarkable stability, maintaining structural and morphological integrity even after 12 h of electrolysis at a current density of 300 mA/cm2. Density functional theory calculation integrated with in situ characterization revealed that synergistic interaction between Cu and Ga enhances the adsorption of key intermediates (*COOH and *CO) and reduces the energy barrier of *CO dimerization. This work provides insights into the design of efficient and stable Cu-based electrocatalysts for C2+ production via an electrochemical method.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121733
·
IF 7.5
Qing Yang,Yanmei Deng,Shuangjiang Li,Xiliang Li,Tingyan Ye,Yi Liu,Yunfei Zhi,Shaoyun Shan
The conversion of CO 2 into cyclic carbonates is crucial for achieving carbon neutrality and enabling resource recycling. Developing efficient heterogeneous catalysts from renewable biomass is a key direction in green catalysis. This study designed a green and efficient heterogeneous catalyst (MCA-PIL) by acetylating bamboo-derived cellulose to construct a porous cellulose acetate support, followed by immobilization of 1-methyl-3-allylimidazolium bromide. The catalyst was systematically characterized using FTIR, XPS, solid-state 13 C NMR etc., which confirmed its chemical structure, hierarchical porosity, and thermal stability. Under optimized conditions (120 ℃, 1.5 MPa CO 2 , 8 h), MCA‑PIL achieved a 99 % yield of chloropropene carbonate from CO 2 and epichlorohydrin without solvent or co-catalyst. The catalyst exhibited broad substrate scope across various epoxides and maintained high activity over five consecutive cycles. Kinetic studies indicated first-order reaction kinetics with an apparent activation energy of 48.35 kJ·mol −1 . Experimental and density functional theory (DFT) analyses revealed a synergistic three-step mechanism: cooperative activation of the epoxide and CO 2 by surface hydroxyl groups and the imidazolium ring, followed by Br - -induced ring-opening, CO 2 insertion, and cyclization to form the product with concurrent catalyst regeneration. This work provides new design principles for biomass‑based catalysts and demonstrates a synergistic strategy integrating CO 2 valorization with renewable material development.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Chen Chi,Xue-Lu Chen,Jian Li,Jin Li,Xing-Hua Xia
Plasmonic nanostructures can utilize solar energy to drive the CO2 conversion. However, noble metals such as gold and silver struggle to mediate multielectron reduction pathways to value-added products. Here, a spatially separated plasmonic–semiconductor hybrid catalyst is designed by coupling MoS2 quantum dots to Au triangle nanoprisms. This hybrid enables hot electrons generated from both interband and intraband transitions in Au to cross over the Au–MoS2 interfacial barrier and inject into MoS2, thereby improving both the selectivity and activity of the electrocatalytic CO2 reduction reaction (CO2RR). The interband hot electrons with energies near the Au Fermi level tend to correlate with the formation of C1 products, selectively enhancing methanol production at low overpotential and promoting formic acid at higher overpotentials; meanwhile, the high-energy intraband hot electrons consistently associate with C–C coupling, significantly increasing ethanol selectivity. These results highlight the unique advantage of spatially separated catalysts in plasmon-mediated electrochemical reactions, providing an approach to utilize interband/intraband hot electrons for efficient and selective CO2RR.
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