CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Shuo Gao,Mengchen Li,Shunlong Xu,Junsu Jin,Jianguo Mi,Hong Meng
Heterometallic Ni/In-gallate was constructed by In 3+ incorporation. • CO 2 gate-opening pressure shifted from 0.10 to 0.07 bar at 298 K. • CO 2 /N 2 selectivity of Ni/In-gallate increased by about 8.5 times. • CO 2 uptake of Ni/In-gallate increased by 91.8% at 0.15 bar. • Ni/In-gallate retained 96.7% (82.15%) CO 2 breakthrough time at 40% (80%) RH. Flexible metal–organic frameworks (MOFs) exhibiting gate-opening transitions are promising for gas separations, yet their performance at low partial pressures is fundamentally constrained by the intrinsic energy barrier governing the structural transition. In this work, In 3+ was incorporated into the Ni-gallate framework to construct heterometallic Ni-O···In motifs. This modification induced localized charge redistribution and enhanced the electrostatic potential gradient within the pore environment. As a result, the gate-opening pressure for CO 2 is shifted from 0.10 to 0.07 bar, accompanied with a significant uptake at 0.15 bar (from 1.83 to 3.51 mmol g −1 ) and IAST selectivity (13287). In situ DRIFTS and kinetic analyses further show a faster establishment of CO 2 adsorption features and a stronger interaction between EPM-Ni/In-gallate and CO 2 . Changes in the electrostatic potential in localized regions within the EPM-Ni/In-gallate were investigated using XAS and PALS measurements. Furthermore, DFT calculations show a substantial reduction in the free-energy barrier for CO 2 migration between adjacent cavities. These results are consistent with a contribution from modified pore-wall polarization and gating energetics. This work identifies electrostatic control as a promising approach for tuning gate-opening transitions in flexible porous materials, providing new design principles for low-pressure gas capture.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Jingli Zhai,Wanting Li,Xinyu Zhang,Qian Zhang,Xiaoqiang Liu,Ruifeng Chong,Caixia Feng,Yan Wang,Danny K.Y. Wong,Yanmei Zhou
Herein, a bimetallic zinc-cobalt metal-organic framework (ZnCoMOF) microsphere cluster with abundant oxygen vacancies was rationally designed and synthesized for visible-light-driven photocatalytic CO 2 reduction. XPS results reveal that the substitution of Co 3 + by Zn 2+ modulated the electronic structure of Co sites, reduced the Co 3+ /Co 2+ ratio, and generated electron-rich Co 2+ centers as well as oxygen vacancies. The reversible Co 3+ /Co 2+ redox pair accelerates charge migration, while oxygen vacancies inhibit carrier recombination. Moreover, electron-enriched Co 2+ favor CO 2 activation. The synergistic effect of multiple active centers optimizes reaction kinetics and catalytic performance. The optimized Zn 0.3 Co 1 MOF delivered a CO yield 2.21 times as high as that of pristine CoMOF, reaching 5.33 mmol g −1 within 4 h, and it achieved an ultrahigh CO selectivity of 100%. The enhanced performance benefits from Zn-induced electronic modulation and synergistic catalysis. Notably, in a diluted CO 2 atmosphere, the product composition exhibits an obvious transition from CO to CH 4 with the decrease in CO 2 concentration. Lower CO 2 concentration contributes to a higher CH 4 yield and greater CH 4 selectivity in the products. Under 20% CO 2 atmosphere, the CH 4 production reached 0.36 mmol g −1 within 4 h with an ultra-high CH 4 selectivity of 100%. These results indicate that in the Zn x Co 1 MOF-catalyzed CO 2 reduction system, product selectivity can be readily modulated by adjusting CO 2 concentration. This offers a facile strategy for the efficient utilization of low-concentration CO 2 from industrial flue gas. Download: Download high-res image (394KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jinhai Leng,Jianqing Wu,Fengying Ma,Weihua Chen,Yinghua Yao,Kunzheng Zhan,Shihao Wu,Qinfen Gu,Shanshan Shang,Daiqi Ye
Direct air capture (DAC) of CO 2 is a critical negative-emission technology for mitigating climate change. Although amine-functionalized metal-organic frameworks (MOFs) are promising DAC adsorbents, their performance is often constrained by inherently limited microporosity, restricted amine loading, and slow mass transfer. Here, we report a novel strategy to engineer hierarchically porous cerium MOFs Ce-BPY (HP-Ce-BPY) by controllably forming defects through specific photoinduced linker distortion and coordination-bond weakening, generating abundant mesopores while preserving structural crystallinity. Subsequent amine grafting markedly strengthens CO 2 affinity, with HP-Ce-BPY-EDA delivering a CO 2 uptake of 1.35 mmol g⁻ 1 at 1.0 bar and 0.25 mmol g⁻ 1 under DAC conditions (0.4 mbar), over 1000-fold higher than pristine Ce-BPY and HP-Ce-BPY. Remarkably, humidity further enhances dynamic CO 2 adsorption, achieving 0.7 mmol g⁻ 1 at 75% relative humidity, while maintaining over 80% capacity after ten adsorption-desorption cycles. Combined CO 2 -TPD and in-situ DRIFTS analyses reveal a chemisorption-dominated, humidity-dependent adsorption mechanism, shifting from carbamate formation under dry conditions to bicarbonate formation in the presence of water, thereby improving amine utilization efficiency and CO 2 uptake. This work introduces a simple, scalable, and cost-effective photochemical route to hierarchically porous amine-functionalized MOFs, offering a promising material platform for high-performance DAC under realistic ambient environments.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Fangzheng Zou,Xianxiang Bai,Hao Wu,Jiguang Li,Lingjun Tan,Xuehua Shen,Zuotai Zhang,Feng Yan
K 2 CO 3 enhances oxidative stability of PEI-based adsorbent without sacrificing CO 2 uptake. • K 2 CO 3 regulates pore confinement and surface acid-base properties of the silica support. • In situ DRIFTS and mass spectrometry reveal suppressed PEI oxidative degradation. • EPR and 1 H NMR confirm reduced radical accumulation and restricted chain mobility. • DFT calculations reveal inhibited hydrogen abstraction by K 2 CO 3 charge regulation. Solid amine adsorbents are promising candidates for CO 2 capture, but their practical application is severely limited by oxidative degradation under high-temperature and oxygen-containing conditions. Conventional strategies mainly rely on chemical modification of amine species, which often compromises CO 2 adsorption capacity or introduces complex synthesis routes. Herein, we report a simple yet effective strategy using K 2 CO 3 as an inorganic additive to enhance the oxidative stability of polyethyleneimine (PEI)-based adsorbents. The introduction of K 2 CO 3 make total PEI content was comparable, but significantly improves CO 2 uptake retention after accelerated oxidation compared with the pristine counterpart. Systematic characterizations reveal that K 2 CO 3 regulates the local microenvironment by tuning pore confinement and surface acid-base properties of the silica support, while modifying the interfacial chemical environment of PEI. In situ DRIFTS and mass spectrometry analyses demonstrate that K 2 CO 3 suppresses the formation of carbonyl/imine-containing intermediates and reduces the evolution of volatile degradation products. Electron paramagnetic resonance and 1 H NMR relaxation results indicate that K 2 CO 3 inhibits radical accumulation and restricts polymer chain mobility. Density functional theory calculations further reveal that K 2 CO 3 reduced the thermodynamic driving force for hydrogen abstraction and modulates local charge distribution at reactive sites, suggesting suppressed radical initiation difficult. This work provides a simple inorganic additive strategy for constructing durable solid amine adsorbents, offering a general design principle for durable CO 2 capture applications under harsh oxidative conditions. Download: Download high-res image (380KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Science Bulletin
·
2026
·
IF 20.7
Juntao Zhang,Di Yan,Shuang Wei,Yihong Chen,Xusheng Wang,Guixiang Ding,Bin He,Ruixia Liu,Li Shuai,Guangfu Liao
Integration of renewable biomass valorization with CO 2 reduction offers a transformative path toward carbon neutrality. However, orchestrating the simultaneous production of high-value 2,5-furandicarboxylic acid (FDCA) and multi-carbon (C 2+ ) chemicals represents a significantly uncharted frontier. Unlike traditional coupling systems, this specific dual-production is severely hampered by the substantial kinetic mismatch and competing reaction pathways, leaving the efficient co-electrolysis of 5-hydroxymethylfurfural (HMF) and CO 2 to high-order products virtually unexplored. Herein, we report a catalyst comprising high-entropy alloy nanoparticles with five elements (Co, Ni, Fe, Cr, Mn) supported on carbon nanofibers (HEA/CNF), which is employed to couple the HMF oxidation reactions (HMFOR) with the CO 2 reduction reaction (CO 2 RR). Endowed with the distinctive electronic structure induced by the high-entropy atomic environment and the collaborative mechanism of multi-site division of labor, the catalyst achieves completely conversion for HMFOR, yielding FDCA with a selectivity of 99.2% and a Faradaic efficiency of 98.8%, surpassing the vast majority of state-of-the-art electrocatalysts reported to date. CO 2 is efficiently reduced to two-carbon (C 2 ) products, which exhibit a Faradaic efficiency of 61.3% at CO 2 RR. Combined in situ spectroscopic analyses and theoretical calculations demonstrate that the Co sites with modulated electronic structures serve as the dominant active centers for the adsorption and HMFOR. The Ni sites assist the reaction via the adsorption of hydroxyl species (OH ads ), while the Fe sites, benefiting from their optimized d-band center positions, act as the key active sites for facilitating the activation of CO 2 and C-C coupling. This work not only presents a high-performance bifunctional high-entropy alloy catalyst, but also uncovers the atomic-scale synergy of its active sites, thereby providing a new design paradigm for integrated biorefining-CO 2 electrocatalysis. Download: Download high-res image (133KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2026
·
IF 7.1
Minggang Guo,Shixin Ma,Xiaohang Yang,Yan Dai,Panpan Mi,Qinzheng He,Huaiyu Sun,Huahao Wang,Hai Liang,Gaohong He
A rigid-flexible interlocked interpenetrating network structure is constructed. • PHMS-AGE/EC blend membranes are fabricated in isopropanol. • The permeability, selectivity, and toughness of EC-based membranes are simultaneously improved. • PHMS-AGE/EC-7:3 shows 588% higher permeability, 14% higher selectivity, and 1046% higher toughness vs. EC. To address the challenge of synergistically enhancing permeability and selectivity in gas separation membranes, a novel green membrane fabrication strategy is proposed. The strategy relies on the synergistic bridging effect of covalent bonds and intermolecular hydrogen bonds between poly(methylhydrosiloxane) (PHMS) and ethyl cellulose (EC). Flexible PHMS is incorporated into the rigid EC network to construct a rigid-flexible interlocked interpenetrating network structure, which reveals a dual-effect regulation mechanism for both separation performance and mechanical properties. The structure forms a synergistic mass-transfer channel that combines the rigid confined sieving property of EC and the flexible high-flux permeation property of PHMS. The results show that the CO 2 permeability, CO 2 /N 2 selectivity, and mechanical ductility of the membrane are simultaneously enhanced. The CO 2 permeability of the PHMS-AGE-1/EC-7:3 membrane reaches 724.3 Barrer, with a CO 2 /N 2 selectivity of 25.5 and an elongation at break of 51.47%. Compared with the EC membrane, the values are increased by 588.14%, 14.40%, and 1046.33%, respectively. Through the design of a rigid-flexible interlocked molecular structure, this work demonstrates excellent separation and mechanical properties, providing innovative insights and theoretical support for low-cost biomass-derived separation membranes applied to industrial flue gas CO 2 capture. To address the challenge of synergistically enhancing permeability and selectivity in polymeric gas separation membranes, a novel green membrane fabrication strategy is proposed. An interlocked network is formed by bridging flexible PHMS with rigid EC via AGE. The CO 2 permeability of the PHMS-AGE/EC-7:3 membrane reaches 724.3 Barrer, with a CO 2 /N 2 selectivity of 25.5 and an elongation at break of 51.47%. Compared with the EC membrane, these values are increased by 588.14%, 14.40%, and 1046.33%, respectively. Different from most EC modification routes requiring costly additives and harmful organic solvents, this preparation method uses fully commercialized raw materials and low-pollution isopropanol, featuring simple operating steps and low comprehensive production cost. This work offers a practical path for developing biomass-based CO 2 separation membranes suitable for industrial application. Download: Download high-res image (174KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Min Li,Juan Li,Tingyan Ye,Shuangjiang Li,Wenjun Zhang,Yutong Zhang,Yunfei Zhi,Pingyan Wang,Donghui Liu,Tianding Hu,Shaoyun Shan,Na Li,Yi Liu
The utilization of CO 2 as a sustainable carbon feedstock is an attractive strategy toward carbon neutrality, while the development of efficient heterogeneous catalysts under mild and co-catalyst-free conditions remains challenging. Herein, three porous organic polymer catalysts (PLZ, PLY, and PL-YZ) were synthesized through a one-step bidirectional polymerization strategy to systematically investigate the individual and synergistic roles of hydrogen-bond donor site (HBDs), Lewis basic N sites, and nucleophilic Cl − sites in CO 2 cycloaddition. Among them, PL-YZ exhibited the highest catalytic activity, affording chloropropylene carbonate in 93.1% yield with nearly 100% selectivity under optimized mild conditions (80 °C, 0.5 MPa CO 2 , 8 h) without any co-catalyst. In addition, PL-YZ maintained over 86% yield after five consecutive cycles and displayed broad substrate applicability toward various terminal epoxides. Kinetic analysis, in situ FT-IR spectroscopy, and DFT calculations consistently revealed that the cooperative interactions among HBD sites, Lewis basic N sites, and nucleophilic Cl − sites promote epoxide activation and ring-opening, facilitate CO 2 insertion, and accelerate cyclic carbonate formation. This study demonstrates the high product yields, selectivity, and recyclability of multifunctional porous polymer catalysts under mild conditions and establishes a practical design principle for integrating complementary active sites toward sustainable CO 2 conversion.
✓ 已验证
产品关联
DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2026
·
IF 5.7
Huijun Wang,Junhai Wang,Xi Chen,Chonghao Yang,Weibin Li,Qihao Jiang,Xingyu Zhan,Hongbin He,Naixu Li,Li Zhang,Jiancheng Zhou
Multicarbon fuel synthesis achieved via photothermal-photocatalytic coupling. • Localized thermal flux synergizes with charge dynamics to accelerate surface kinetics. • Pt loading minimizes carrier recombination and maximizes solar-to-chemical efficiency. The integration of photothermal and photocatalytic processes presents a promising pathway to boost solar-driven CO 2 conversion, yet achieving efficient photo–heat synergy under concentrated sunlight remains challenging. Here, we report a Pt-nanoparticle-decorated WO 3 catalyst fabricated via chemical reduction, which demonstrates exceptional activity for CO 2 reduction under concentrated solar irradiation. The optimized 0.8Pt/WO 3 catalyst achieves CO, CH 4 , and C 2 H 4 production rates of 4.12, 2.12, and 0.63 μmol·h −1 ·g −1 , respectively, with a noteworthy 25.8- and 28.3-fold enhancement in CO and CH 4 yields upon switching from unconcentrated to concentrated light. Systematic characterization reveals that Pt nanoparticles not only act as electron sinks to facilitate charge separation and interfacial transfer, but also enhance visible-light absorption and photothermal conversion. Under concentrated irradiation, the coupled photothermal effect elevates the local temperature to ∼405 °C, promotes high-density carrier accumulation, and significantly lowers the apparent activation energy from 21.21 to 13.80 kJ·mol −1 . This work elucidates a synergistic photothermal–photocatalytic mechanism where enhanced charge dynamics and localized heating jointly drive efficient CO 2 valorization, offering a design blueprint for high-performance solar fuel catalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xu Chen,Yanlei Liang,Ying Zhang,Jun Wang,Junzhong Wang,Zhengkun Yang,Xifan Chen,Juan-Ding Xiao,Jia Yang
2, 2′-bipyridine-modified copper realizes CO 2 electroreduction to C 2+ products. • Excellent performance with a maximum C 2+ Faradaic efficiency of 70%. • Asymmetric catalytic sites promote OC-COH coupling, driving C 2+ production. Electrochemical reduction of CO 2 to value-added multi‑carbon (C 2+ ) products represents a promising technology for sustainable chemical synthesis and environmental remediation. However, achieving highly efficient CO 2 electroreduction toward C 2+ products remains challenging due to the high energy barriers inherent to carbon‑carbon (C C) coupling. Herein, we report a 2, 2′-bipyridine-modified copper catalyst with asymmetric catalytic sites (bipyridine-modified Cu sites and adjacent bare Cu sites), which exhibits exceptional selectivity with low overpotential for CO 2 electroreduction to C 2+ products. The catalyst achieves a maximum C 2+ Faradaic efficiency of 70% at −0.64 V vs. RHE in a gas-diffusion flow cell, significantly enhanced compared with copper catalyst without 2, 2′-bipyridine (51%). Mechanistic investigations reveal that the copper sites modified by 2, 2′-bipyridine facilitate the formation of *COH intermediate, while adjacent bare copper sites realize *CO formation. Furthermore, the asymmetric catalytic sites promote OC-COH coupling, thereby overcoming the high energy barrier inherent to C C coupling and effectively driving C 2+ production. Our work establishes asymmetric catalytic sites engineering as a strategic paradigm for advancing CO 2 -to-C 2+ conversion catalysts. A 2, 2′-bipyridine-modified copper catalyst enables asymmetric C C coupling between *CO and *COH intermediates, achieving efficient CO 2 -to-C 2+ conversion. Download: Download high-res image (116KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yinying Shu,Songqi Li,Yuquan Li,Cheng Zheng,Xiaogang Yang,Yahui Cai,Zhengying Wu,Jundie Hu,Jiafu Qu
Interfacial engineering enables Pd 0 /oxygen vacancy balance in Pd/In 2 O 3 . • Hollow In 2 O 3 nanotubes moderate Pd-In 2 O 3 metal-support interaction. • Pd/h-In 2 O 3 achieves 8020 mmol FA mol Pd −1 h −1 for formate production. • Pd 0 retention and defect accessibility jointly govern formate formation. The catalytic performance of oxide-supported Pd catalysts in CO 2 hydrogenation is highly dependent on the interfacial cooperation between metallic Pd 0 sites and defect-containing oxide domains. However, how to regulate this metal-oxide interfacial balance to simultaneously promote H 2 activation and CO 2 -derived intermediate conversion remains insufficiently understood. Herein, we develop an interfacial engineering strategy to regulate the balance between metallic Pd 0 sites and oxygen vacancies (Ov) in Pd/In 2 O 3 catalysts through morphology-dependent metal-support interaction (MSI). Structural analyses reveal that hollow In 2 O 3 nanotubes (h-In 2 O 3 ) effectively moderate Pd-In 2 O 3 interactions, preserve a higher fraction of metallic Pd 0 , and maintain accessible defect-associated oxide domains, thereby establishing a more favorable interfacial configuration than compact counterparts. Consequently, Pd/h-In 2 O 3 delivers the highest formate production rate of 8178 ± 145 mmol FA mol Pd −1 h −1 at 60 °C and 2 MPa, representing a sixfold enhancement over rod-like Pd/In 2 O 3 (Pd/r-In 2 O 3 ), together with excellent stability. These findings highlight that the coordinated regulation of metallic-site preservation and defect accessibility is critical for constructing efficient metal-oxide interfaces for CO 2 hydrogenation to formate. Interfacial engineering optimizes the Pd 0 /Ov balance in Pd/In 2 O 3 by moderating metal-support interaction, enabling high formate productivity (8178 ± 145 mmol FA mol Pd −1 h −1 ) in CO 2 hydrogenation. Download: Download high-res image (147KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Jing Li,Fan Zhang,Peng Zhang,Guowei Niu,Shanshan Liu,Huichuang Guo,Fei Wang,Qiang Chang,Hong Wang,Chenghua Zhang,Yong Yang,Yongwang Li
Si 3 N 4 is proposed as a precursor to construct Fe-Si interactions in FTS catalysts. • Fe/Si 3 N 4 catalyst exhibits stronger Fe-Si interaction and higher Fe 2 SiO 4 content than Fe/SiO 2 . • The formation of Fe 2 SiO 4 stabilizes Fe species and suppresses the formation of Fe 3 O 4 . • Preventing the formation of Fe 3 O 4 makes for decreasing CO 2 selectivity and WGS activity. Precise control over the metal-support interfacial structure plays a critical role in enhancing the activity and selectivity of iron-based catalysts for syngas conversion. Using silicon nitride as the starting precursor of silicon support, a series of SiN x O y supports with different oxidation degree were constructed via controlled oxidation under air, enabling modulation of the Fe-Si interfacial environment. A systematic comparison between silicon nitride-derived supports and conventional silica support revealed significant differences in structural evolution and catalytic behavior of iron catalysts. Spectroscopic characterizations including FTIR, solid-state NMR, XPS, XRD, and Mössbauer spectroscopy demonstrated that the unique interfacial structure formed during the oxidation of Si 3 N 4 stabilizes the active iron species (carbides) and suppresses the formation of undesired phases (Fe 3 O 4 ), thereby reducing CO 2 selectivity. These findings underscore the critical influence of support precursors on interfacial chemistry and reaction pathways, providing new insights and strategies for the rational design of Fe-based catalysts. Download: Download high-res image (76KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2025
·Vol. 92
·期 1
·127-138
·
IF 2.6
Wang Wei,Li Haoxuan,Xie Yue,Zhao Yingying,Xiong Rihua
Climate change demands innovative carbon capture and utilization (CCU) strategies, yet converting captured CO 2 into high-value products while managing industrial waste remains elusive. Here, we demonstrate a single-step, energy-efficient bipolar membrane electrodialysis (BMED) system integrated with CCU, enabling the simultaneous conversion of NaCl brine and CO 2 into high-purity sodium bicarbonate (NaHCO 3 ) with unprecedented efficiency, but without requiring external alkali sources or energy-intensive thermal regeneration steps. By optimizing key parameters – such as current density and CO 2 aeration rate, and gas–liquid flow ratios – we achieved a bicarbonate concentration of 1.186 mol/L in the alkaline chamber, coupled with 57.65% carbon sequestration efficiency and an energy consumption as low as 3.1 kW·h/m³ CO 2 (or 716.9 kW·h/t NaHCO 3 ). This approach not only recovers valuable sodium resources from brine but also enhances CO 2 absorption through electrochemical mechanisms, potentially reducing global carbon emissions by up to 20% in brine-intensive industries. Our work paves the way for scalable, sustainable CCUS technologies, transforming waste streams into economic assets and advancing the fight against climate change. Integration of BMED with CO 2 sequestration for NaHCO 3 production from NaCl brine. Energy-efficient and sustainable CO 2 utilization for marketable products. Optimization of key operational parameters for improved efficiency.
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）