CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Hang Yao,Jian Sheng,Jie Fan,Hong-Mei Jiang
The selective hydrogenation of CO 2 to either CH 4 or CO is a pivotal reaction for sustainable chemical synthesis, yet controlling product selectivity remains challenging. Although Ru-based catalysts are highly active for CO 2 methanation, their selectivity to CO is typically low. Herein, we demonstrate that gallium oxide (GaO x ) serves as an efficient promoter for Ru/Al 2 O 3 catalysts, switching the dominant product in ambient-pressure CO 2 hydrogenation from ∼98% CH 4 to ∼92% CO. Comprehensive characterization reveals that GaO x engages in a strong electronic metal-support interaction with Ru, which facilitates electron transfer from Ru to Ga, generating electron-deficient Ru sites that weaken CO adsorption. In situ DRIFTS further demonstrates that Ga redirects the reaction pathway from a dual mechanism favoring CH 4 formation on Ru/Al 2 O 3 to a selective route producing CO via formate intermediate decomposition. This work provides fundamental insights into how oxide promoters can steer reaction pathways through electronic effects and offers a rational strategy for designing selective CO 2 hydrogenation catalysts.
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JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 8.8
Yuting Zhang,Qian Sun,Bizi Yu,Weiwang Lim,Ayan Yao,Jingcheng Du,Yumo Fan,Xuan Ding,Daijun Meng,Wen He,Ji Ma,Jian Guan,Hongjun Zhang,Jiangtao Liu
Mixed matrix membranes (MMMs) incorporating metal-organic frameworks (MOFs) hold great promise for energy-efficient carbon capture, yet are fundamentally limited by interfacial defects and the ubiquitous permeability-selectivity trade-off. Herein, we propose a nanoconfinement strategy via in-situ interfacial polymerization to synthesize ultrathin MOF nanosheets and thus integrate them into PIM-1 matrix, a typical representative of polymers of intrinsic microporosity (PIMs), crafting a defect-free membrane. The meticulously designed MOFs, featuring synergistic amino functionalities and unsaturated Cu 2+ sites, endows the optimal membrane (PIM-MOF-1%) with exceptional CO 2 affinity and tailored molecular-sieving pathways. Consequently, it achieves a remarkable combination of high CO 2 permeability (5186 barrer) and CO 2 /N 2 selectivity (41), surpassing the 2019 Robeson upper bound. Impressively, this superiority persists under harsh conditions-exceeding the 2008 Robeson upper bound at 80 °C and sustaining high performance at 15 bar. Moreover, the membrane demonstrates exceptional long-term durability, preserving excellent separation performance, with CO 2 permeability of 3078 barrer and CO 2 /N 2 selectivity of 46, even after 180 days of aging. Our strategy aligns nanoconfined MOF architectures with polymer matrix, thereby resolving critical challenges in carbon capture through the simultaneous enhancement of separation efficiency and durability.
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JOURNAL OF CATALYSIS
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2026
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IF 6
Xinping Duan,Jinlin Lu,Zhaojun Wen,Xuelian Liang,Haiqiang Lin,Linmin Ye,Youzhu Yuan
In supported metal catalysis, conventional strong metal-support interaction (SMSI) often leads to the encapsulation of active metal sites, thereby suppressing catalytic performance, for instance, nickel-based in thermocatalytic CO 2 hydrogenation. Here, we demonstrate that constructing a defective TiO x overlayer on anatase TiO 2 via room-temperature NaBH 4 treatment effectively transforms the classical SMSI state into a quasi-reactive metal-support interaction (quasi-RMSI) in Ni/TiO 2 -based catalysts. This pre-engineered interface, abundant in Ti 3+ and oxygen vacancies, prevents the formation of a dense TiO x encapsulation layer while facilitating electron transfer to Ni nanoparticles and promoting the activation of both CO 2 and H 2 . As a result, the Ni catalyst exhibits a one-order-of-magnitude increase in the CO 2 methanation rate with nearly 100% CH 4 selectivity, a 12-fold enhancement in turnover frequency, and exceptional long-term stability over 200 h. Combined spectroscopic and microscopic analyses reveal that the quasi-RMSI creates a highly active and accessible Ni-TiO x interface, which significantly accelerates CO 2 dissociation and sequential hydrogenation. This work establishes a general defect-engineering strategy for designing high-performance CO 2 methanation catalysts via tailored quasi-RMSI.
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Journal of Materials Chemistry A
·
2026
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IF 9.2
Jinglin He,Ziheng Jin,Rui Zhou,Zhongde Dai,Hui Su,Yiqiao Zhang,Bangda Wang,Xia Jiang
The urgent demand for efficient CO2 capture from high-temperature flue gas streams necessitates the development of advanced adsorbents with robust structural stability and rapid sorption kinetics. While amine-functionalized materials offer promising affinity for CO2 within elevated-temperature operational windows, conventional post-loading strategies often compromise pore accessibility and hinder mass transfer due to network obstruction. Here, we introduce an innovative in situ self-assembly approach to incorporate amine functionalities directly into the interconnected meso- and macroporous framework of carbon supraparticles (CSs). This strategy takes advantage of hydroxyl-rich carbon nanofibers (CNFs) during in situ synthesis to help retain amines within the CS pores and anchor them more strongly to the support, leading to amines showing a more uniform distribution, and better resistance to evaporation and leaching. The resulting material demonstrates rapid CO2 uptake at 1 bar and 70 °C, achieving an impressive adsorption rate of 0.17 mmol g−1 min−1 and a capacity of 2.87 mmol g−1, while exhibiting appropriate adsorption stability over repeated adsorption–desorption cycles. These performance metrics represent 4-fold and 2.4-fold enhancements in rate and capacity, respectively, compared to conventional post-loading approaches. Overall, this work presents a scalable and sustainable strategy for developing high-efficiency CO2 capture materials suited for industrial deployment.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Weitao He,Chun Miao,Wei Jiang,Li Yan,Chunbo Liu,Keyu Cui
Photocatalysis, which represents a clean and efficient energy conversion technology, shows great potential for addressing both environmental pollution and the energy crisis. Within this context, photocatalytic CO 2 reduction and pollutant degradation represent important research directions. In this study, CdIn 2 S 4 /g-C 3 N 4 (g-C 3 N 4 , graphitic carbon nitride) composites were hydrothermally synthesized and assessed for their photocatalytic performance in the reduction of CO 2 and the degradation of methyl orange and tetracycline as model pollutants. Among the synthesized composites, the optimal photocatalytic activity was achieved by the CdIn 2 S 4 /g-C 3 N 4 (80) composite, with the degradation efficiency for methyl orange reaching 97.21% over 100 min and the reduction efficiency for CO 2 reaching 74.34 μmol g −1 over 4 h. The obtained results demonstrated that the heterojunction formed between CdIn 2 S 4 and g-C 3 N 4 effectively promoted the separation of photogenerated charge carriers while effectively suppressing their recombination, thereby improving the photocatalytic performance. Moreover, a cyclic stability experiment demonstrated that the CdIn 2 S 4 /g-C 3 N 4 composite exhibited excellent recyclability, which is important for its practical application. This work therefore provides a promising strategy for the design of highly efficient and stable photocatalysts toward sustainable environmental remediation and energy conversion.
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Small
·
2026
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IF 11.8
Junhui He,Zhansheng Wang,Jiang Xue,Bichu Huang,Linjuan Yang,Cong Luo,Xudong Cui,Zhuoyu Ji,Daopeng Sheng,Tao Chen,Wenkun Zhu
Surface halogen atom modification represents a promising strategy for regulating the photocatalytic performance of covalent organic frameworks (COFs). In this study, a surface bromine atom modification strategy is proposed for TzPm-COF material, which finely tunes its donor-acceptor (D-A) structure and significantly enhances both the activity and selectivity of CO 2 photoreduction. By virtue of the in situ Kelvin probe force microscopy (KPFM), along with others spectral technology we confirm that bromine functionalization effectively facilitates the separation and migration of photogenerated charge carriers. Accordingly, the as-prepared TzPm-COF-2Br exhibits a remarkable CO production rate of 155 µmol g − 1 h − 1 under visible-light-driven CO 2 reduction, approximately 2.7 times higher than that of TzPm-COF (57 µmol g − 1 h − 1 ), along with exceptional selectivity (99.4%), which surpasses the majority of analogous CO-producing photocatalysts in overall performance. Relying on the functional theory (DFT) calculations, we further confirm the introduction of bromine atoms promoted directional electron transfer from TAPTz donors to PMDCA-2Br acceptors through intrinsic polarization effects, thereby enhancing the adsorption and activation of CO 2 at oxygen sites on PMDCA units. This work provides a rational material design strategy for developing functionally modified COFs toward efficient and selective photocatalytic CO 2 reduction.
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CHEMICAL ENGINEERING & TECHNOLOGY
·
2026
·Vol. 49
·期 6
·e70256
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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
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2026
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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
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2026
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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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
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2026
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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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ACS Catalysis
·
2026
·Vol. 16
·期 17
·17145-17155
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IF 13.6
He Ye,Liu Huiyu,Sheng Jianping,Du Chenyu,Moghadam Majid,Sun Yanjuan,Dong Fan
Halide perovskite nanocrystals are promising photocatalysts for CO 2 reduction due to their strong light absorption, defect tolerance, and tunable excited-state properties, but their practical performance remains limited by tightly bound excitons, rapid charge recombination, and inefficient interfacial electron delivery. Here, we report an anthraquinone (AQ)-modified CsPbBr 3 nanocrystal photocatalyst (CPB/AQ) in which the redox-active π-conjugated AQ ligand functions as an interfacial electron relay and molecular electric-field modulator. Experimental and theoretical analyses collectively reveal that AQ creates an additional interfacial charge-transfer pathway, strengthens the light-induced surface potential difference from 170 to 270 mV, and decreases the exciton binding energy from 44.05 to 40.74 meV. Consequently, CPB/AQ achieves a CO yield of 433.50 μmol g –1 within 3 h under AM 1.5G irradiation, 4.54 times that of pristine CPB, and maintains stable CO evolution during a 25 h test. Isotopic 13 CO 2 tracing verifies that CO originates from CO 2 reduction, while in situ FTIR spectroscopy demonstrates enhanced CO 2 adsorption/activation and accelerated formation of *COOH and *CO intermediates on CPB/AQ. This work highlights molecularly gated interfacial electric-field regulation as an effective strategy for overcoming charge-transfer bottlenecks in perovskite nanocrystal photocatalysis.
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