TRANSACTIONS OF TIANJIN UNIVERSITY
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2026
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IF 7.8
Lei Ling,Wang Jiaxiang,Tian Feng,Yin Mingjie,Wang Wentao,Li Mengna,Dong Liangliang
The detection of trace antibiotics in aquatic environments poses a critical global challenge, threatening both ecological safety and public health. Forward osmosis (FO) membrane separation technology has emerged as a highly efficient approach for purification of trace antibiotics, characterized by high treatment efficiency and low energy consumption. However, challenges inherent to the recycling of draw solutions restrict the development of FO technology. Herein, we report the synthesis and application of a novel CO 2 -responsive SiO 2 @PDEA nanocomposite as a highly recyclable particulate draw solution. This system leverages CO 2 /heat-triggered reversible switching between hydrophilicity and hydrophobicity to enable facile recovery. The 6 wt% SiO 2 @PDEA solution leads to a significantly enhanced water flux ( J w ) to 5.31 LMH (PRO mode), a threefold increase over bare SiO 2 . Crucially, the ratio of reverse solute flux ( J s ) to J w was minimized to 0.015 g/L, providing a substantial cost advantage over inorganic salts. The efficiency of this approach enabled a threefold concentration of tetracycline. Furthermore, the solution demonstrated outstanding cyclic stability with a solute recovery rate consistently exceeding 99% via mild thermal stimulation. These findings demonstrate that SiO 2 @PDEA is an exceptionally efficient, sustainable, and cost-effective draw solution with substantial potential for the practical remediation of trace antibiotic-containing wastewater.
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Nature Communications
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2026
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IF 18.1
Liu Zheyang,Mao Liang,Liu Yifan,Nie Kaiqi,Zhou Min,Yan Binhang,Jiang Zhifeng,Shi Weidong,Liu Bin
Photocatalytic CO 2 -to-ethanol conversion offers an interesting route for intermittent solar energy utilization. However, the performance is impeded by slow mass-transfer and high dimerization barrier (>1.0 eV) of *CO intermediates, coupled with a kinetic mismatch between the short-lived carriers and the 12 e⁻ reaction. Herein, we develop a Z-scheme Cu δ+ O/floral-like BN photocatalyst that achieves CO 2 -to-ethanol conversion with near 100% selectivity. The photocatalyst utilizes the three-dimensional structure and alkaline surface of BN to concentrate CO 2 and directs transfer of long-lived carriers to unsaturated Cu⁺ sites, stabilizing them for flexible electron donation to the π* orbital of CO 2 . Enhanced ethanol photosynthesis activity/selectivity stems from a new pathway: CO 2 is first reduced to HCOOH at Cu δ+ O sites, lowering the C–C coupling barrier to 0.44 eV. Liquid formate is then concentrated and protonated to C 2 precursor, minimizing side reactions for high selectivity. Here, we show the feasibility of selective ethanol photosynthesis and uncovers a new formate intermediate pathway.
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Gas Science and Engineering
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2026
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IF 6.8
Zhihao Zhang,Mingwei Zhao,Zhongzheng Xu,Zhixue Sun,Yingnan Wang,Yizheng Zhang,Huan Zhang
CO 2 dry fracturing technology offers advantages such as environmental friendliness, mitigation of water-sensitive damage, and improved flowback efficiency, making it an ideal choice for the development of low-permeability and tight unconventional reservoirs. However, the inherently low viscosity of liquid CO 2 limits its proppant-carrying and fracture-propagating capacity. The introduction of efficient thickeners is currently the most effective method. In this work, an ester-modified polysiloxane polymer (PDH) was successfully synthesized via the copolymerization and hydrosilylation, its dissolution and thickening mechanisms in liquid CO 2 were systematically investigated using high-pressure phase equilibrium experiments combined with molecular dynamics simulations. Experimental results showed that both the cloud pressure and thickening performance of PDH in liquid CO 2 improved significantly with increasing thickener and co-solvent concentrations. At a thickener dosage of 5 wt% and co-solvent (ethanol) dosage of 5 wt%, PDH exhibited a cloud pressure of only 10.91 MPa and increased the viscosity of liquid CO 2 by 59.02 times. Simulation results indicate that strong dipole–quadrupole interactions between the polar ester groups and CO 2 enhance compatibility can reduce intermolecular distances and increase interaction energies. Furthermore, the higher rigidity of PDH chains and the formation of a stable solvation layer effectively restrict CO 2 mobility, leading to significantly lower mean square displacement and diffusion coefficients compared to PDMS. These features enable PDH to achieve high solubility and pronounced thickening effects at relatively low pressures. It can provide theoretical support for the synthesis and screening of CO 2 thickeners in the future.
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Particuology
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2026
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IF 4.7
Yi Zhang,Liangwei Hu,Yuan Lu
The escalating atmospheric CO 2 concentration calls for advanced carbon capture solutions. However, developing a stable and efficient adsorbent with high selectivity for CO 2 capture remains a significant challenge. Microporous materials capture CO 2 primarily through physisorption based on pore structure and van der Waals forces. In this study, three silicon-aluminum zeolite molecular sieve materials were synthesized and hydrophilic modification of ZIF-8 was achieved through post-synthetic coordination with polyethylene glycol. A systematic comparison of the CO 2 adsorption performance of these materials under different conditions was then conducted. Zeolites exhibited exceptional thermal stability (< 5% mass loss from 25-800 °C under an air atmosphere) and cyclability (retaining > 95% of initial adsorption capacity throughout cycling), outperforming ZIF-8 analogues. 85-nm zeolite achieved the optimal CO 2 uptake (1.8 mmol g -1 ) at 25 °C and ZIF-8 showed the best humidity resistance (40% decrease at 80% RH). Additionally, ZSM-5 exhibited enhanced gas retention of 1498 s, indicating superior CO 2 adsorption affinity. These results demonstrate the excellent thermal stability and cycling stability of the zeolite materials. This study provides actionable insights for future material design: 1) prioritizing zeolite-based frameworks for scenarios requiring long-term cyclic stability and thermal robustness; 2) optimizing pore size and surface properties to balance adsorption capacity and selectivity; 3) developing anti-poisoning modifications targeting SO 2 competitive adsorption in flue gas.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Faisal Irshad,Dan Zhang,Hamzah A.S.M. Yaseen,Xianming Zhu,Muhammad Chawla,Shengping Wang,Yongli Shen,Xinbin Ma
Pd/H-MOR exhibits superior catalytic activity and stability for CO 2 hydrogenation to formateover other Pd/Zeolites and M/H-MOR. • Brønsted acid sites at Pd-H-MOR interface polarize CO 2 , while highly dispersed Pd nanoparticles dissociate H 2 barrierlessly. • Low Si/Al ratio optimizes metal-support synergy and reducing apparent activation energy to HCOOH. • Bicarbonate identified as the key reaction intermediates by in-situ DRIFTS and DFT study. Catalytic hydrogenation is a promising route for CO 2 conversion, yet the highly efficient formation of formic acid remains challenging. Herein, Pd nanoparticles dispersed on mordenite (Pd/H-MOR) are reported as an efficient and stable catalyst for CO 2 hydrogenation to produce formates. Under optimized conditions, Pd/H-MOR achieved an intrinsic turnover number of 1828 and a turnover frequency of 914 h −1 at 120 °C, surpassing all the other prepared catalysts with different metal active sites and zeolite supports. The high activity arises from the co-effect of Pd and the H-MOR support: Pd sites dissociate H 2 into active hydrogen, while Brønsted acid sites enhance CO 2 adsorption via polarization and stabilize bicarbonate intermediates, which subsequently convert to formates. Density functional theory (DFT) results revealed that Pd/H-MOR lowers the activation barriers for both H 2 dissociation and CO 2 activation at the Pd-MOR interface and combined with in-situ DRIFTS, identifying surface bicarbonates as the key reactive intermediates en-route to formate formation. Comparatively, kinetic studies of Pd/H-MOR revealed a reduced apparent activation energy of 15.81 ± 0.79 kJmol −1 , reflecting strong metal-support interactions, while the observed R = k ∙ P CO 2 0.56 ∙ P H 2 0.62 reaction orders indicate that the reaction rate is weakly dependent of H 2 and CO 2 pressures but strongly dependent on the nature of the metal and the zeolite support. This work highlights metal dispersion and support acidity as key factors for CO 2 hydrogenation. Download: Download high-res image (224KB) Download: Download full-size image
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Nature Communications
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2026
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IF 18.1
Zhang Shaowei,Wang Shuo,Liu Hewei,Zou Geng,Guo Yige,Zhang Wenwen,Yu Lina,Liu Haolin,Zhang Xiaomin,Li Mingrun,Zhang Peng,Yu Runsheng,Zheng Xusheng,Song Yuefeng,Wang Guoxiong,Bao Xinhe
Single-atom catalysts (SACs) offer high atomic efficiency and catalytic activity but are prone to aggregation and degradation under high-temperature conditions. Here, we propose a thermally and electrochemically stable high-valent iridium single atom synthesis strategy based on strong metal-support interactions (SMSI) to enhance high-temperature CO 2 electrolysis performance in solid oxide electrolysis cells (SOECs). The SMSI effect, in situ induced during high-temperature cell fabrication and operation, stabilizes the high-valent iridium single atom and simultaneously modulates the surface electronic structure of the La 0.6 Sr 0.4 FeO 3−δ (LSF) cathode by weakening the Fe−O hybridization, finally promoting oxygen vacancy formation and enhancing CO 2 adsorption and activation. This approach boosts the CO 2 -to-CO electrolysis current density by 80.8% relative to the pristine LSF cathode, achieving 3.02 A cm −2 at 800°C and 1.5 V with nearly 100% Faradaic efficiency and excellent stability over 600 h. These findings provide a viable strategy for designing thermally and electrochemically robust SACs for high-temperature catalytic reactions.
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Nature Communications
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2026
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IF 18.1
Huang Zhongnian,Wang Jundi,Ge Xiaohu,Lang Junyu,Cao Yueqiang,Wan Ying,Qian Gang,Yang Yong,Zhou Xinggui,Chen De,Yuan Weikang,Duan Xuezhi
CO 2 hydrogenation over earth-abundant Ni catalysts is attractive for CO-based fuel synthesis, but Ni intrinsically favors methanation. Here we show that ordered Ni 3 Sn 2 intermetallics tune Ni–CO electron back-donation and switch CO 2 hydrogenation from CH 4 formation to the reverse water–gas shift reaction. Atomic-resolution microscopy and X-ray absorption spectroscopy reveal disruption of extended Ni–Ni ensembles by Sn, while spectroscopy and theoretical calculations show that Ni–Sn d - p hybridization downshifts the Ni 3 d band and weakens Ni→CO 2π* back-donation. The Ni 3 Sn 2 catalyst achieves CO 2 conversion approaching thermodynamic equilibrium with nearly 100% CO selectivity and remains stable for 300 h. In situ infrared spectroscopy, steady-state isotopic transient kinetic analysis and theoretical calculations indicate that H-assisted CO 2 activation, spectator-like formate species and facile CO desorption underpin the CO-selective pathway. Similar behavior over Ni–Ga and Ni–In catalysts suggests a general back-donation strategy for redirecting Ni-based CO 2 hydrogenation.
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ACS Catalysis
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2026
·Vol. 16
·期 16
·16055-16065
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IF 13.6
Wang Yanlin,Gu Panpan,He Ruoyan,Xue Qizhou,Cheng Aofei,Liu Xiang,Zeng Shaojuan,Wang Min,Zhang Zhenlei,Zhang Kaihang,Feng Jiaqi,Zhang Xiangping
The electrochemical CO 2 reduction reaction (CO 2 RR) is a proton−electron coupled transfer process in which active hydrogen (*H) plays a pivotal role in determining the reaction pathways, particularly for methane (CH 4 ), a representative deep hydrogenation product. However, how *H generation and migration govern CH 4 formation remains elusive, motivating mechanistic elucidation to enable rational regulation of reverse hydrogen spillover. Herein, we develop Cu-doped ZrO 2 catalysts and reveal that tuning the crystallinity of the ZrO 2 support enables control over the reverse hydrogen spillover process. Specifically, amorphous ZrO 2 functions as an efficient “hydrogen pump” by promoting *H generation and lowering the migration barrier toward adjacent Cu sites, thereby strengthening the reverse hydrogen spillover effect. This effect establishes an optimal *H coverage for deep hydrogenation of CO 2 , thereby reducing the energy barriers for key intermediates along the CH 4 formation pathway. Consequently, the Cu-doped amorphous ZrO 2 catalyst delivers a CH 4 Faradaic efficiency of 69.3% with a partial current density of −372.8 mA cm −2 , significantly surpassing that of its crystalline analogue. This work highlights that engineering the crystallinity of metal oxide supports provides an effective strategy to regulate reverse hydrogen spillover in electrocatalysis, offering valuable insights into controlling catalytic activity and product selectivity.
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ACS Catalysis
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2026
·Vol. 16
·期 17
·17380-17391
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IF 13.6
Ma Meifeng,Zhang Rongwang,Deng Shaorong,Zhao Xilai,Yang Fei,Fang Xiuzhong,Wang Xiang,Xu Xianglan
Rational design of highly active catalysts for low-temperature CO 2 methanation remains a critical challenge for efficient CO 2 utilization. Herein, we demonstrate that Mn incorporation into the Cr 2 O 3 lattice, rather than surface modification, markedly enhances the catalytic performance of Ru/Cr 2 O 3 catalysts. The optimal Ru/Mn 0.10 Cr 0.90 O x catalyst (2.24 wt % Ru) achieves 91% CO 2 conversion at 200 ° C with a space velocity of 36,000 mL g cat –1 h –1 , substantially exceeding that of the parent Ru/Cr 2 O 3 (4% at 200 ° C). Compared with Ru/Cr 2 O 3 , Ru/Mn 0.10 Cr 0.90 O x exhibits a 4.1-fold higher turnover frequency at 180 ° C, confirming the intrinsic catalytic enhancement conferred by Mn lattice doping. Comprehensive characterization revealed that Mn lattice doping generates Mn-O-Cr bonds, creating distinct Ru/O-Cr-O v -Mn interfacial sites in contrast to the Ru/O-Cr-O v -Cr interfaces present in undoped Ru/Cr 2 O 3 . In situ DRIFTS and H 2 -TPSR-MS studies demonstrated that low-temperature CO 2 methanation on Ru/Mn 0.10 Cr 0.90 O x proceeds concurrently via both CO* and HCOO* intermediate pathways, whereas only the CO* pathway operates on Ru/Cr 2 O 3 . DFT calculations revealed that Mn doping selectively modulates CO 2 adsorption at the interface while minimally affecting bridged Ru sites. At the Ru/O-Cr-O v -Mn interface, oxygen vacancies form and regenerate more readily than at the Ru/O-Cr-O v -Cr interface during CO 2 methanation, enabling an additional HCOO* pathway. This dual-pathway mechanism fundamentally underpins the enhanced low-temperature activity of Ru/Mn 0.10 Cr 0.90 O x and provides a promising design strategy for developing efficient CO 2 methanation catalysts.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2026
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IF 7.1
Wenzheng Hou,Duoyong Zhang,Jiarui Ji,Xinnan Cui,Huashan Bao,Chen Zhang,Liwei Wang
Polymer-mediated strategy enables AlFum with regulated pore structure. • Microporous domains are enhanced while the AlFum framework remains intact. • The optimized AlFum achieves a 25.5% higher CO 2 uptake at 0.15 bar. • Sorption heat of the materials remains far below typical amine-loaded sorbents. The compact crystallization and dense particle aggregation of aluminium fumarate (AlFum) may limit the effective utilization of its intrinsic microporous sorption domains for CO 2 capture. To address these limitations, a pore-structure regulation strategy is developed by employing polyethyleneimine as a transient polymeric modulator during the synthesis of AlFum. Unlike conventional amine-loading strategies that enhance CO 2 affinity through retained amine-rich phases but may sacrifice microporosity and increase sorption energetics, this approach is associated with dosage-dependent changes in particle assembly and textural pore development while preserving the intrinsic AlFum framework. The optimized AlFum(PEI-0.2) delivers the best CO 2 sorption performance among the series, with a 25.5% uptake enhancement at 0.15 bar. Despite the improved capacity, it maintains a moderate isosteric heat of 21–25 kJ mol −1 , consistent with predominantly physisorption-based and reversible CO 2 sorption. Delayed CO 2 breakthrough and increased dynamic CO 2 uptake under 15% CO 2 /85% N 2 demonstrate enhanced dynamic CO 2 retention for AlFum(PEI-0.2), while five consecutive breakthrough cycles at 30% RH retain 96.6% of the first-cycle uptake. GCMC simulations further identify the intrinsic micropores of ideal AlFum as preferential equilibrium CO 2 sorption domains. This strategy establishes a pore-structure design enabled by transient polymeric modulation, balancing intrinsic microporous domains with textural pore development and providing a promising route toward stable Al-based MOF adsorbents for CO 2 capture. Download: Download high-res image (213KB) Download: Download full-size image
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GREEN CHEMISTRY
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2026
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IF 10.6
Minzhi Ma,Mengge Jia,Shichu Zhao,Zhiqiang Jiang,Kangle Lv,Tongqing Li,Helei Chai,Yan Lei,Jingjing Si,Zhi Zheng,Wenjun Fa
The global imperative for carbon-neutral fuels starkly contrasts with the persistent failure to achieve solar-driven CH4/C2H6 synthesis from CO2/H2O with both high selectivity and yield, as the thermodynamic propensity for CH4/C2H6 formation collides with kinetic bottlenecks inherent in the multi-electron/proton-transfer cascade. The prevailing paradigm has long posited that CH4/C2H6 selectivity is predominantly governed by reaction kinetics rather than thermodynamics, consequently steering catalyst design toward precise modulation of reactant interfacial dynamics at catalytic surfaces. Contrary to previous assumptions, our study demonstrates for the first time that CO2 photoreduction exhibits a characteristic domino-like chain reaction mechanism: when the catalyst amounts in the reaction system reach the threshold, the reaction cascade preferentially proceeds toward thermodynamically favorable CH4 formation through low-barrier pathways, with even C2H6 generation emerging. The universality of this mechanistic paradigm has been rigorously validated across archetypal catalysts (TiO2, MoO3, CeO2, Ni/CeO2, etc.), revealing that low amounts (5.0 mg) selectively yield H2 and CO (＞60 %, 2e- transfer), whereas higher amounts (200.0 mg) drive product distribution toward thermodynamically favorable CH4 (＞50 %, 8e- transfer). To probe this mechanism, the widely utilized Ni/CeO2 was selected as the benchmark photocatalyst, where the primary constituent of the reduction product shifts from CO/H2 (＞80 %) to CH4/C2H6 (＞80 %) upon increasing Ni/CeO2 amounts. Employing quasi in situ XPS and D2O kinetic isotope effects experiments, we unveil that Ni/CeO2 suprathreshold amounts (>150 mg) create electron-enriched microenvironments at interfacial Niδ+ sites, which drive domino photoreduction of CO2 to CH4/C2H6, while kinetically quenching competing CO/H2 evolution via proton-transfer/CO-desorption impedance. Consequently, this study elucidates that the prerequisite for designing catalysts to resolve the persistent activity-selectivity trade-off is to ensure that the photogenerated carrier concentration at the active site reaches the minimum threshold required for CH4/C2+ generation.
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ACS Applied Materials & Interfaces
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2026
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IF 7.8
Jing Zhao,Yangning Zhang,Tuo Wang,Peng Zhang
The electrochemical CO2 reduction reaction (CO2RR) provides a renewable avenue to convert CO2 to value-added fuels and chemicals. Bismuth (Bi)-based electrocatalysts are known as promising candidates for CO2RR to formate (HCOO–), yet their performance is frequently limited by structural reconstruction during operation, resulting in reduced activity and selectivity. This work describes a thermal treatment approach to tuning the catalytic chemistry of α-Bi2O3 for CO2RR. A thermally optimized Bi-400 electrocatalyst achieves a high Faradaic efficiency of 93.0% for HCOO– at −0.95 V vs RHE, along with good stability over 70 h. Through detailed structural and mechanistic studies, it is revealed that the preserved Bi–O motifs in Bi-400 facilitate CO2 activation and modulate the binding energy of the *OCHO intermediate, thereby enhancing both activity and selectivity toward HCOO– production. This study would provide an in-depth understanding of the selective formation of HCOO– products on Bi-based electrocatalysts in CO2RR.
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