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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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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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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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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ACS Nano
·
2026
·
IF 17.3
Shiqun Wu,Chenggui Zhong,Lijie Wang,Ruijie Yang,Ziwei Ye,Chengxuan He,Mingyang Li,Jinlong Zhang
Selective photocatalytic reduction of CO2 to CH3COOH is highly desirable but hindered by poor intermediate stabilization and sluggish C–C coupling. Here we report a coordination-environment engineering strategy to construct asymmetric Co active sites and induce intrinsic spin polarization by nitrogen incorporation into Co3O4. Nitrogen substitution and oxygen vacancy formation generate Co sites with distinct coordination and charge distributions, stabilizing *CO intermediates and lowering the C–C coupling barrier. Concurrently, spin polarization enhances charge carrier separation, further intensified by an external magnetic field. In situ spectroscopy and theoretical calculations confirm the synergistic role of asymmetry and spin effects in facilitating intermediate formation and CH3COOH production. The optimized N–Co3O4–X catalyst achieves a CH3COOH yield of 41.4 μmol g–1 h–1 with 95% electron selectivity under external magnetic field. This work presents a dual-modulation strategy for efficient CO2-to-C2 conversion.
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ACS Applied Nano Materials
·
2026
·
IF 5.8
Luoning Li,Xiaozhuo Zhao,Guocan Jiang,Jinlin Yin,Sheng Li,Zhengquan Li,Jin Wang
Heavy-metal-free photocatalysts for solar-driven CO2 reduction represent a sustainable pathway toward carbon-neutral fuel production. Ternary chalcogenide AgInS2 (AIS) quantum dots (QDs), nanoscale semiconductors (typically 2–5 nm) whose optoelectronic properties are intrinsically governed by quantum confinement and high surface-to-volume ratios, offer an environmentally benign alternative but suffer from insufficient reduction potential and rapid charge recombination. In this work, we demonstrate that Ga3+ doping into AIS (AIGS) QDs simultaneously engineers band edges and suppresses defect-mediated charge recombination. Systematic compositional tuning of AIGS QDs yields optimized photocatalytic CO2 reduction performance, achieving CH4 and CO production rates of 16.7 μmol g–1 h–1─a 6.2-fold improvement over pristine AIS QDs. Combined spectroscopic, electrochemical, and density functional theory investigations establish that Ga3+ doping upshifts the conduction band minimum to enhance thermodynamic driving force while reducing defect states that serve as recombination centers. Transient spectroscopy confirms prolonged charge-carrier lifetimes in AIGS QDs, directly correlating with improved photocatalytic performance. This integrated band engineering and defect passivation strategy provides an efficient way for designing high-performance, heavy-metal-free QD photocatalysts for artificial photosynthesis.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Guowei Chen,Yang He,Shen Xiang,Yiping Zhao,Li Chen
Oxygenation membranes for extracorporeal membrane oxygenation systems require ultrathin, defect-free selective layers that simultaneously deliver high gas permeability, selectivity, and operational stability. Herein, we report a Janus composite membrane featuring a dense polydimethylsiloxane (PDMS) selective layer integrated with a hydrogen-bonded organic framework (HOF-TGU-307), designed to overcome filler aggregation and transport limitations commonly encountered in ultrathin mixed-matrix membranes. A Marangoni convection-driven assembly strategy induces strong in-plane flow at the gas–liquid-solid interface, enabling uniform dispersion and horizontal embedding of HOF crystallites within the PDMS matrix. Theoretical analysis and molecular dynamics simulations confirm that Marangoni flow suppresses capillary-driven aggregation, while a stable PDMS-HOF interfacial network forms polar gas-transport pathways and promotes interfacial CO 2 enrichment. As a result, the optimized M3-HOF membrane exhibits a high single-gas CO 2 permeance of 1883 GPU and an ideal CO 2 /O 2 selectivity of 5.2, measured at 0.1 MPa and 25 °C, together with an oxygen transfer rate of 219.8 mL·min −1 ·m −2 . The Janus architecture further provides excellent interfacial stability, effectively preventing liquid penetration (LEP > 0.6 MPa). Auxiliary evaluations demonstrate reduced protein adsorption and favorable blood-contacting compatibility, supporting its potential for membrane oxygenators. This computation-guided, Marangoni-driven fabrication strategy offers a scalable route for constructing high-performance oxygenation membrane with controlled ultrathin selective layers.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yuanwen Shi,Zhenyu Zhao,Hong Li,Xin Gao
Hot spots (δT = 13–40 °C) on adsorbents during MW heating were quantified. • Localized hot spots accelerated the desorption rate by 18%. • Influences of microwave power and N 2 rates on desorption efficiency were studied. • Cyclic regeneration efficiency was improved by 49% using microwave technology. Temperature swing adsorption (TSA) for CO 2 capture generally suffers from slow thermal response and high energy demand during adsorbent regeneration. Microwave swing adsorption (MSA) has emerged as a promising alternative to enable fast regeneration of CO 2 adsorbents. However, the mechanism of microwave-enhanced desorption remains unclear due to the difficulty in determining the actual surface temperature of adsorbents under microwave irradiation. This challenge is overcome in this study by coating a temperature-sensitive fluorescence thermometer onto the adsorbent particles, confirming the existence of a temperature difference (δT) between the adsorbent surface and the bulk bed measured by a fiber-optic sensor. Subsequently, a convective heat transfer model coupled with an electromagnetic heating equation was established to quantitatively predict the influence of purge flow rate and microwave power on δT. The model predictions agree well with the results of systematic experiments with an error < 20%, revealing that MSA can achieve a desorption efficiency at a bulk temperature of 88 °C comparable to that of conventional TSA at 100 °C, therefore reducing the specific regeneration energy consumption by 55% (to 1.91 MJ/kg CO 2 ) and nearly doubling the cyclic processing efficiency. The quantification of hotspot effect drives rational regulation of microwave enhanced CO 2 desorption, thereby advancing the development of energy-efficient carbon capture technologies.
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Nanoscale
·
2026
·
IF 5.2
Linlong Hu,Chentao Wang,Huibin Wang,Hua Pan,Mi Yan,Ke Wang,Pengfei Xie
CO2 reduction to light olefins is an important pathway toward carbon neutrality, but it is hindered by low thermodynamic conversion and the inherent trade-off between activity and selectivity. To address this challenge, a bifunctional catalyst consisting of Cu single atoms anchored on ZrO2 and SAPO-34 (Cu1/ZrO2-SAPO-34) was developed. This catalyst achieves 84.3% light olefin selectivity and 15.0% CO2 conversion, with stable performance maintained over 100 hours. In this catalyst, Cu single atoms, ZrO2, and SAPO-34 exhibit clear division of labor and synergy, responsible for CO2 activation, active site stabilization, and olefin selectivity control, respectively. Mechanistic investigations using in situ DRIFTS and DFT calculations demonstrate that the interaction between Cu single atoms and ZrO2 facilitates the further hydrogenation of formate intermediates to methoxy species, while reducing the energy barrier for methoxy hydrogenation to methanol, thus ensuring high light olefin selectivity in subsequent conversion over SAPO-34. This work provides new insights for CO2 conversion and the design and application of single-atom catalysts in tandem catalytic reactions.
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AICHE JOURNAL
·
2026
·
IF 4.4
Ziheng Li,Wenji Zheng,Fengting Yao,Zhixu Yun,Yan Dai,Xuehua Ruan,Miao Yu,Tiantian Li,Xiaobin Jiang,Xuemei Wu,Gaohong He
Constructing vertically aligned, penetrating metal–organic framework (MOFs) gas transfer pathways within mixed matrix membranes (MMMs) is an effective strategy for optimizing gas transport under low filler loading (≤25 wt.%). Herein, we developed a novel “stack-polymerize-section” process to construct vertically aligned ZIF-8 pathways in MMMs by tailoring the density and channel size of PAN@ZIF-8 NFM for optimizing CO 2 ultrafast and in-parallel transport. The designed XLPEO/PAN@ZIF-8 MMM exhibits excellent performance far exceeding the 2019 McKeown upper bound, with CO 2 permeability and CO 2 /N 2 selectivity of 369.2 Barrer and 90.0, respectively. Meanwhile, a novel parallel computational model that synergistically integrates the Maxwell model with resistance-based (RB) model methodology was proposed to introduce the interfacial resistance coefficient derived from polymer–MOFs interface heterogeneous concentration gradients. This work demonstrates the potential of vertically aligned MOFs channels for high-performance gas separation, providing a scalable and controllable fabrication pathway for maximizing the efficiency of MOFs in membrane technology.
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