APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Siyu Yi,Guobin Zhou,Yi Wang,Mengxia Ji,Jinman Yang,Yi Zhang,Pengcheng Yan,Zhao Mo,Zhaolong Wang,Junjie Yuan,Hui Xu,Xiaojie She
Electrocatalytic CO 2 methanation is promising for carbon neutrality but hindered by complex multi-electron transfer process, thereby obtaining low product selectivity. Herein, we report a copper single atom catalyst anchored on nitrogen doped carbon nanotubes (Cu-N-CNTs) for efficient electrocatalytic CO 2 methanation. By synergistically regulating the precursor, Cu-N 4 active sites are precisely constructed at the atomic scale, effectively suppressing copper aggregation. In situ characterization indicates that the catalyst forms a moderate local alkaline microenvironment during the reaction, suppressing C-C coupling side reactions and promoting methane pathways. In the flow cell, Cu-N-CNTs achieve a FE CH4 of 59.2% and a partial current density of 168.7 mA cm −2 at −1.577 V vs. RHE, and operated stably for 10 h. Moreover, Cu-N-CNTs exhibit remarkable methane selectivity in membrane-electrode assembly (MEA) systems employing both alkaline and pure-water electrolytes. A scaled-up MEA prototype further verifies the outstanding operational stability of Cu-N-CNTs under practical conditions. These results collectively underscore the substantial potential of Cu-N-CNTs for industrially relevant electrocatalytic CO 2 methanation.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiamin Wang,Fei Liu,Yanqiu Shi,Yizhou Wang,Shangyan Zhou,Xiaodan Wang
CuAl 2 O 4 -derived ZnO/Cu catalyst is constructed via reduction-exsolution and H 2 -SMSI • Precise prereduction control creates rich and active ZnO x /Cu interfacial sites • ZnO x /Cu interface promotes H 2 activation, m-HCOO ⁎ pathway and suppresses RWGS • Superior methanol performance originates from enhanced ZnO x /Cu interfacial synergy • The STY of methanol reaches to 525.8 mg CH₃OH ·h −1 ·g cat −1 and selectivity is close to 75.8% Constructing highly exposed Cu/ZnO interfaces represents a crucial strategy for achieving efficient CO 2 hydrogenation to methanol. In this work, CuAl 2 O 4 spinel was employed as the precursor, and an inverse catalyst (oxide/metal, which is a reverse structure to the traditional metal/oxide catalyst) featuring abundant ZnO x /Cu interfacial sites was obtained by combining reduction-exsolution with a hydrogen-induced strong metal–support interaction (SMSI) strategy. Under the reaction conditions of 240 °C and 3.0 MPa, the optimal ZnO/CuAl 2 O 4 –500 exhibits significantly higher methanol selectivity (75.8%) and space-time yield (525.8 mg CH₃OH ·h −1 ·g cat −1 ) compared to the ZnO/CuAl 2 O 4 with negligible ZnO x /Cu interfacial sites. Multiple characterizations combined with theoretical calculations reveal that the strong electronic interaction at the ZnO x /Cu interfacial sites induces the formation of Cu + species and oxygen vacancy (O v )-rich ZnO x . This markedly enhances H 2 activation and spillover, promotes the generation of highly active monodentate formate (m-HCOO ⁎ ) intermediates, and lowers the energy barrier for methanol formation. Concurrently, the interface suppresses the reverse water–gas shift (RWGS) pathway on Cu 0 sites, thereby improving methanol selectivity. This study presents a controllable synthetic strategy for constructing high-performance inverse ZnO x /Cu interfacial sites, providing new insights for the development of efficient catalysts for CO₂ hydrogenation to methanol. In this work, CuAl 2 O 4 spinel was employed as the precursor, and an inverse catalyst featuring abundant ZnO x /Cu interfacial sites was obtained by combining reduction-exsolution with a hydrogen-induced strong metal–support interaction (SMSI) strategy. Under the reaction conditions of 240 °C and 3.0 MPa, the optimal ZnO/CuAl 2 O 4 –500 exhibits significantly higher methanol selectivity (75.8%) and space-time yield (525.8 mg CH₃OH ·h −1 ·g cat −1 ) compared to the ZnO/CuAl 2 O 4 with negligible ZnO x /Cu interfacial sites. Multiple characterizations combined with theoretical calculations reveal that the strong electronic interaction at the ZnO x /Cu interfacial sites induces the formation of Cu + species and oxygen vacancy (Oᵥ)-rich ZnO x . This markedly enhances H 2 activation and spillover, promotes the generation of highly active monodentate formate (m-HCOO ⁎ ) intermediates, and lowers the energy barrier for methanol formation. Concurrently, the interface suppresses the reverse water–gas shift (RWGS) pathway on Cu 0 sites, thereby improving methanol selectivity. Download: Download high-res image (127KB) Download: Download full-size image
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Energies
·
2026
·Vol. 19
·期 7
·1782
·
IF 3.9
Xiaochen Zhang,Zhihong Li,Ming Li,Yong Zhao,Liang Xu,Yun Zhang,Xiaobin Nie,Lei Tang,Yuanqiang Zhu
Excessive CO2emissions cause global warming, while CO2interaction with crude oil can enhance oil recovery (EOR). To capture and reuse CO2, nano-SiO2was cationically modified to synthesize nanoparticles (SCR2). The structure and performance of SCR2were characterized by FT-IR, DLS, and TEM, confirming its excellent CO2adsorption capacity and surface activity. Compared with unmodified nano-silica, SCR2increased CO2adsorption capacity by 254.3% and reduced the core surface contact angle from 112.1° to 24.5°. Core flooding experiments showed that in low-permeability reservoirs, SCR2achieved a plugging rate of 87.5%, an enhanced oil recovery of 24.8%, and an ultimate oil recovery of 74.8% (23.8% higher than unmodified nano-silica). Mechanistically, SCR2plugs gas channeling pathways via its inherent nanoparticle properties and adsorption of dissolved CO2in the aqueous phase while improving rock surface wettability, thereby enhancing sweep efficiency and total oil recovery during CO2flooding. This study provides a promising approach for EOR and CO2resource utilization in low-permeability reservoirs.
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Small
·
2026
·
IF 11.8
Zhenliang Zhu,Jianfei Xiao,Ruiyao Li,Yaoqi Huang,Shaojun Yuan
Ultramicroporous MOFs capable of simultaneously separating C 2 H 6 /C 2 H 4 and C 2 H 2 /CO 2 mixtures remain rare due to the stringent requirements on pore confinement and adsorption-site distribution. Here, we report a dual-ligand engineered porphyrin-based framework, Zn-TCPP-mtz, constructed from Zn 2+ nodes, tetrakis(4-carboxyphenyl)porphyrin (TCPP), and 5-methyl-1H-tetrazole (mtz). The incorporated mtz ligands bridge adjacent porphyrin layers and, together with interlayer hydrogen-bonding interactions, result in a compact stacking arrangement featuring 1D ultramicropores (7.2 × 4.8 Å 2 ) decorated with N/O functional sites and hydrophobic methyl groups. This tailored pore environment enables Zn-TCPP-mtz to adsorb 2.63 and 2.56 mmol g −1 of C 2 H 6 and C 2 H 4 , respectively, as well as 3.14 and 1.89 mmol g −1 of C 2 H 2 and CO 2 at 298 K and 1 bar, achieving selectivities of 1.5 for C 2 H 6 /C 2 H 4 and 3.1 for C 2 H 2 /CO 2 . Dynamic breakthrough experiments confirm one-step production of high-purity C 2 H 4 (>99.9%) and C 2 H 2 (>99.5%) with productivities of 3.0 and 16.3 L kg −1 , respectively. DFT calculations reveal that the ultramicroporous channels provide well-defined interaction sites that stabilize C 2 H 6 over C 2 H 4 and C 2 H 2 over CO 2 through multiple dispersion-dominated contacts. This study demonstrates that the dual-ligand strategy can be extended to construct porphyrin-based frameworks with controlled pore architectures and stable adsorption environments, enabling the integration of multiple C 2 gas separations within a single material platform.
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高影响因子
ACS Applied Energy Materials
·
2026
·
IF 5.5
Xinran Huang,Tao Ma,Ronggui Yu,Qinghe Xiao,Qi Liu,Jianpeng Dong,Huitao Fan,Liya Wang,Bo Li
Utilizing solar energy to achieve photocatalytic CO2 reduction represents a potential method for CO2 conversion. As an emerging semiconductor material, metal halide perovskites offer advantages such as a broad light absorption range, long carrier lifetime, and tunable energy band, demonstrating good application prospects in the field of photocatalysis. CsPbBr3 (CPB) is a representative metal halide perovskite, possessing stable active sites and excellent photocatalytic activity. However, CPB tends to suffer from structural instability in certain environments, and its high carrier recombination rate leads to inadequate photocatalytic performance. To address these issues, we loaded CsPbBr3 quantum dots (CPB QDs) onto porous polygonal tubular carbon nitride (PCN) to construct a CPB-CN composite photocatalyst with a type-II heterojunction, which enables efficient photocatalytic CO2 reduction. Compared with pristine CPB QDs, the CPB-CN heterojunction significantly enhances carrier separation. By further optimizing the CPB-CN ratio, the optimal 20% CPB-CN composite photocatalyst exhibited improved photocatalytic reduction performance and charge separation efficiency. The CO2-to-CO reduction rate reached 20.94 μmol g–1 h–1, almost 3-fold of pure CPB. The improved photocatalytic properties can be ascribed to efficient electron extraction and migration at the interface of PCN and CPB QDs, the high specific surface area, and enhanced visible-light harvesting. This work demonstrates the potential for the design of highly catalytically active perovskite-based systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Shumei Li,Yijie Wang,Yameng Wang,Maobin Wei,Xin Li,Binrong Li,Lili Yang
All-inorganic CsPbBr 3 perovskite quantum dots (QDs) are promising photocatalysts for CO 2 reduction, but their application is limited by aggregation and photoinduced instability. Herein, a 2D/0D BiOBr/CsPbBr 3 S-scheme heterojunction was constructed by anchoring CsPbBr 3 QDs on BiOBr nanosheets. The 2D BiOBr support promotes uniform QD dispersion and exposes more accessible active sites. More importantly, the intimate interface establishes an internal electric field that favors directional interfacial charge transfer in an S-scheme configuration. This pathway facilitates the depletion of photogenerated holes from CsPbBr 3 while retaining strongly reductive electrons for CO 2 conversion, thereby improving charge separation and contributing to enhanced photostability. The optimized composite delivers CO and CH 4 evolution rates of 170.4 and 33.0 μmol g −1 h −1 , respectively, corresponding to 3.8- and 3.2-fold increases over pristine CsPbBr 3 QDs, together with improved cycling stability. XPS, UPS, KPFM, photoelectrochemical measurements, in situ FTIR spectroscopy, and DFT calculations collectively support the S-scheme mechanism and reveal a lower Gibbs free-energy requirement for COOH* formation. These synergistic effects account for the enhanced photocatalytic activity and stability. Download: Download high-res image (150KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yuehua Zhang,Jiyuan Zhang,Songrui Wang,Mingjin Yang,Xin Meng,Yun Zhao,Jiaxuan Liu,Yuqiong Kang,Shanshan Luo,Hao Du,Shuangyu Jiang,Wenglam Wong,Hongyi Kang,Dazhi Li,Baohua Li,Bing Li,Haiping Xu
In/C-0.2 achieves 93.5% Faradaic efficiency for formate at -0.6 V vs. RHE with 400 mV overpotential and 80 h operation. • Indium dispersion regulates CO 2 adsorption and electron transfer, enabling low-overpotential formate production. • TOF-SIMS combined with FT-IR reveals that In sites promote *OCHO formation and suppress competing pathways. • Electronegativity-driven charge polarization stabilizes O-bound *OCHO and facilitates highly selective formate formation. Electrochemical CO 2 reduction to formate is limited by high overpotentials and competing reactions. Herein, we report an indium single-atom catalyst that modulates the adsorption geometry of CO 2 by engineering the charge state of the active site. The optimized catalyst achieves a Faradaic efficiency (FE) for formate of 93.5% at −0.6 V vs. RHE in a flow cell with 400 mV overpotential and maintains high selectivity across a wide potential window (-0.6 to −0.9 V). The overpotential of formate is highly sensitive to the initial dispersion of In atoms causing optimal CO 2 adsorption and fast electron transfer, and increases significantly when In clusters/particles become predominant species. In situ characterizations and theoretical calculations indicate that oxygen-coordinated isolated In sites induce significant interfacial charge polarization, which preferentially stabilizes a bidentate O-bound adsorption configuration of CO 2 -derived intermediates through strong In-O interactions and thereby enables highly selective conversion to formate. This work identifies electronegativity as a key descriptor for controlling intermediate adsorption on p-block single-atom catalysts and provides insights into the rational design of selective CO 2 RR electrocatalysts. Download: Download high-res image (296KB) Download: Download full-size image
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Science Advances
·
2026
·Vol. 12
·期 31
·
IF 13.9
Kun Li,Yuan Peng,Wentai Hu,Xinyu Wang,Weishen Yang
Carbon capture is essential for producing blue hydrogen and syngas. However, designing a single membrane with dual CO 2 -selective and H 2 -selective separations has long been considered impractical because these modes rely on fundamentally different mechanisms. We report a stimuli-responsive membrane that overcomes this limitation by integrating two functional materials. A zirconium metal-organic polyhedron (Zr-MOP) polymerized hydrogel membrane was fabricated via a stepwise molecular-level blending and polymerization strategy, achieving excellent filler dispersion, strong interfacial compatibility, and good solution processability. The Zr-MOP cages reinforce the hydrogel hydrogen-bond network, enabling high CO 2 -philic performance with a CO 2 /H 2 separation factor of 44 and CO 2 permeability of 7025 Barrer. Upon dehydration, membrane shrinkage induces cage rearrangement and exposure of molecular sieving windows, switching the separation behavior to a highly H 2 -selective mode with an H 2 /CO 2 separation factor of 798. This transition is reversible and can be further regulated by pH stimuli. This work introduces a strategy for membranes with switchable and inverted separation functions.
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Current Organocatalysis
·
2026
·Vol. 13
·期 2
·152-162
·
IF 1.1
Guangyu Zhang,Ningkun Xu,Feng Sun,Bing Sun,Xinmei Liu,Wei Xu,Zhe Yang
Introduction The catalytic cycloaddition of CO2 with epoxides to produce cyclic carbonates represents one of the most promising CO2 utilization technologies, offering 100% atomic economy under mild conditions. Nevertheless, the development of cost-effective heterogeneous catalysts with high performance under solvent- and cocatalyst-free conditions remains a grand challenge. Herein, we report the rational design and synthesis of a multifunctional heterogeneous catalyst for efficient CO2/propylene oxide (PO) cycloaddition under solvent- and cocatalyst-free conditions. Methods The ZnMgAl-Br- heterogeneous catalyst was prepared through an integrated coprecipitation-ion exchange method. Structural and physicochemical properties were systematically characterized using SEM, XRD, EDX mapping, BET, and NH3-TPD, which confirmed the coexistence of abundant Br- nucleophiles and –OH hydrogen-bond donors within the layered matrix. Catalytic tests were conducted in a 50 mL stainless steel autoclave. Results A Br- intercalated ZnMgAl layered double hydroxide (ZnMgAl-Br-) catalyst was successfully constructed, integrating nucleophilic Br- anions with hydrogen-bond donating –OH groups in a precisely engineered layered framework. Under optimized conditions (140oC, 7 h, 2.5 MPa), the catalyst achieved 99.2% PO conversion, 98.7% PC selectivity, and 97.9% PC yield. The result represents a remarkable improvement compared with benchmark catalysts (MgAl-Br−: 50.5% yield; ZnMgAl-NO3−: 13.1% yield), highlighting the critical synergy among Br- nucleophiles, Zn species, and –OH groups. Discussion The results demonstrate that the cooperative interaction between Br- and –OH groups is central to the catalytic efficiency of CO2/PO cycloaddition. Incorporation of Zn species expanded the interlayer spacing and optimized the spatial arrangement of Br−/-OH sites, thereby enhancing cooperative catalysis. Conclusion The findings highlight the critical role of Br- nucleophiles and the Zn-modified layered structures in enabling cooperative catalysis. This work establishes a rational strategy for designing multifunctional heterogeneous catalysts for efficient CO2 utilization through epoxide cycloaddition.
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 35
·20411-20420
·
IF 4.6
Qin Mingxin,Ye Yuanyuan,Zhang Mengjie,Li Zhiming,Chen Yang,Yao Fanglei,Chen Ziheng,Wu Qikang,Hu Zhi,Yue Sisi,Niu Weichao,Li Feng,Zhang Cheng,Wang Jin
Electrochemical CO 2 reduction reaction (CO 2 RR) enables sustainable conversion of CO 2 into
high-value
fuels and chemicals, yet precise selectivity control toward methane
(CH 4 ) and multicarbon (C 2+ ) products remains
difficult. Herein, we develop a cyclic voltammetry (CV)-triggered
electrochemical reconstruction strategy to modulate the CO 2 RR selectivity of Cu-LDH-derived catalysts. Tailoring the CV potential
window and cycle number effectively tunes the catalyst microstructure
and copper (Cu) valence state: narrow potential windows with limited
cycles produce grain-boundary-rich Cu particles with low-valence sites,
which promote *CO accumulation and C–C coupling to yield a
high C 2+ Faradaic efficiency (FE) of 83.3% at 400 mA cm –2 . In comparison, expanded potential windows with prolonged
cycling induce the formation of nanoclusters with abundant high-valence
Cu sites, which suppress C–C coupling and favor the sequential
deep hydrogenation of adsorbed *CO intermediates, achieving a CH 4 FE of 64.7% at 300 mA cm –2 . Ex situ characterizations and in situ spectroscopic
analyses reveal that CV-driven dissolution–redeposition dominates
the evolution of particle size, grain boundaries, and Cu valence,
thereby governing the CO 2 RR reaction pathways. This work
establishes a facile electrochemical reconstruction strategy for programmable
modulation of CO 2 RR product selectivity.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 34
·15374-15386
·
IF 7.6
Li Chenguang,Zhou Mingjun,Li Yuchen,Wang Xue,Wang Lei,Fang Cheng,Wu Gongde,Ding Jing,Wan Hui,Guan Guofeng
Direct conversion of CO 2 into ethanol represents a promising route toward carbon neutrality. In this study, a series of Zr-modified K-FeCu/MWCNT catalysts were developed for efficient and selective CO 2 hydrogenation to ethanol. The introduction of Zr promoted ethanol formation primarily by diversifying the reaction pathways toward ethanol and enhancing the dispersion of active phases. The electronic interactions among Zr, Fe, and Cu significantly reduced the particle sizes of the Fe and Cu phases and effectively restrained their migration and agglomeration. Furthermore, ZrO 2 served to adsorb and activate in situ generated CO, which subsequently coupled with CH x * species on the Fe 5 C 2 surface to yield C 2+ oxygenated intermediates, thereby favoring ethanol formation. Under the reaction conditions of 320 ° C, 4 MPa, and 6000 mL·g cat –1 ·h –1 , the Zr-modified K-FeCu/MWCNT catalyst exhibited a 44.39% higher space-time yield (STY) of ethanol than its unmodified counterpart. This performance considerably surpasses that of most Fe-based catalysts reported to date, providing insights and design strategies for developing high-performance catalysts for CO 2 hydrogenation to ethanol.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Haozhan Chu,Guoxiong Zhan,Kuilin Peng,Yinge Bai,Pengfei Gao,Hongyu Zhang,Zehua Wei,Xiangping Zhang,Shaojuan Zeng
Ionic liquids (ILs) show great potential for carbon dioxide (CO2) capture due to their designable structures and dual roles as absorbents and catalysts. Our previously designed IL solvent ([Cho][Triz]/TMS) showed good absorption performance but a slow regeneration rate. Here, a novel strategy to promote CO2 desorption in IL absorbents at lower temperatures using homogeneous Lewis acid IL (LAIL) catalysts was proposed. The cobalt (Co)-based LAIL [Bmim]2[CoCl4] exhibited superior performance, with the CO2 desorption amount enhanced by 54.1% and activation energy reduced by 30.3% compared with the blank test, leading to low regeneration energy consumption (0.90 GJ/t CO2), which was ascribed to a simultaneous increase in Brønsted and Lewis acid sites, promoting C–N bond cleavage by C2–H in [Bmim]22+ and Co sites in [CoCl4]2–. The environmental impact of IL-based CO2 capture processes, evaluated by the green degree method, demonstrated that the green degree production value of the IL-LAIL system is 79.6 and 673.6 gd/h higher than that of the IL and MEA systems, respectively, indicating greater environmental sustainability. This study provides a viable strategy for employing homogeneous catalysts to facilitate energy-efficient CO2 capture.
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