JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.7
Xin Li,Ze Lv,Tong Wu,Bolin Ji,Wei Wu,Yi Zhong,Hong Xu,Zhiping Mao,Linping Zhang
Enhancing the photocatalytic CO 2 conversion efficiency of metal-organic frameworks (MOFs) remain a central challenge in advancing carbon capture and utilization (CCU) technologies. Herein, we report a mixed-ligand strategy to construct a hybrid MOF (denoted as CTN ⊂ NM) by incorporating a Co-metalated tetrakis(4-carboxyphenyl)porphyrin (CoTCPPNa 4 , CTN) into an amine-functionalized MIL-101(Fe) framework (NH 2 -MIL-101(Fe), abbreviated as NM; MIL = Materials of Institute Lavoisier, a prototypical series of robust MOFs). The optimized catalyst with a Co/Fe molar ratio of 0.40 achieves a HCOOH production rate of 119.11 μmol g −1 h −1 under visible light in the absence of a sacrificial agent, representing a 4.2-fold increase compared with pristine NM. When a sacrificial electron donor is introduced, the rate further rises to 179.87 μmol g −1 h −1 . The markedly enhanced activity originates from the synergistic integration of CTN and NM: CTN provides strong visible-light absorption and efficient catalytic sites, while NM offers high porosity and strong CO 2 affinity. This cooperation broadens the light-absorption range, suppresses charge-carrier recombination, and accelerates CO 2 -reduction kinetics. In addition, the Co 3+ center in the metalloporphyrin macrocycle functions as an active CO 2 adsorption site, facilitating its activation and selective conversion to HCOOH. Overall, this study presents an effective mixed-ligand hybridization approach for solar-to-chemical energy conversion and provides valuable insights for the rational design of MOF-based photocatalysts toward carbon-neutral fuel production.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF RARE EARTHS
·
2026
·
IF 7.2
Shaohong Guo,Ruyue Zheng,Huimin Yu,Jiaqi Yan,Jiayu Li,Haobo Wen,Ziyun Zhou,Jingchun Jia,Ying Chang,Meilin Jia,Changyan Zhu,Heng Jia,Jiang Wang,Zhongmin Su
Photocatalytic CO 2 reduction into value-added chemicals such as CO is of great importance for carbon-neutral in the future. However, both high CO 2 activation barriers and sluggish charge kinetics make it still a challenge for CO 2 photoreduction with high reactivity. Herein, a type-II heterojunction (CZ/C), which consists of CdS (C) nanospheres anchored on the defective Ce-doped ZnIn 2 S 4 (CZ) microflowers, was synthesized by an in-situ solvothermal route, realizing exceptional CO 2 catalytic performance under simulated sunlight irradiation. According to the detailed characterizations and density functional theory calculations, the energy barrier of the rate determining step is significantly reduced due to the outstanding CO 2 adsorption and activation on rare earth Ce atoms. Simultaneously, the separation and transfer efficiency of photogenerated carriers are greatly facilitated by type-II heterojunction constructed by anchoring CdS on CZ and S vacancies resulting from a heteroatom doping strategy. Thus, the optimum photocatalyst of CZ2/C2 composite provides an advantageous platform for CO 2 photoreduction to CO, which is roughly 7.5- and 3.0-fold higher than those of the pristine ZIS and CZ2, respectively. This work offers a promising avenue for designing effective catalysts with a dual-strategy method for photocatalysis.
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2026
·
IF 16
Yong Su,Junli Xu,Jia Zhao,Congcong Du,Qiunan Liu,Jiwei Li,Sixu Liu,Zhun Zhang,Yang Luo,Lin Geng,Jingzhao Chen,Kelvin H. L. Zhang,Yongfu Tang,Liqiang Zhang,Qiao Huang,Kazu Suenaga,Feiteng Wang,Jun Cheng,Sen Lin,Wei Tan,Lin Dong,Fudong Liu,Jianyu Huang,Haifeng Xiong
Metal single-atom catalysts (SACs) offer exceptional atomic efficiency and remarkable properties, making them highly valuable for energy and environmental applications. However, existing SAC preparation methods face challenges, such as the need for high temperatures or limitations in metal loading. In this study, we present a room-temperature synthesis strategy for stable SACs with high metal loadings (>10 wt %), achieved through electrochemical redox reactions within lithium-ion batteries. The reaction mechanism was thoroughly elucidated, revealing that bulk metallic compounds (denoted as MaXb, where M represents a metal and X is F, S, or O) disintegrate from the millimeter scale down to single atoms at room temperature. This process is driven by lithiation–delithiation-induced grain refinement and the dissolution of metals, which are subsequently captured by the substrate. The resulting single-atom catalyst (e.g., Cu SAC) demonstrates outstanding reactivity for electrocatalytic CO2 reduction, showcasing excellent electrochemical stability and superior performance. This room-temperature redox method is versatile and compatible with a wide range of metals and supports, highlighting its potential for broad applications in sustainable catalytic technologies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Carbon Neutrality
·
2026
·Vol. 5
·期 1
·4
·
IF 12.5
Wang Shaona,Yang Yang,Xu Wenqing,Bai Zhuoshu,Su Fabing,Wang Yixi,Bai Dingrong,Zhu Tingyu
As an integrated CO 2 capture and utilization (ICCU) process, direct electrochemical reduction of amine captured-CO 2 reduction reaction (cCO 2 RR) has enormous advantages in energy efficiency and operating cost. The low product selectivity is an urgent issue. Here, we found that the hydroxyl (-OH) on CeO 2 can significantly enhance CO selectivity. After hydroxyl modification, the CO faraday efficiency (FE CO ) was surprisingly increased by 188% (relative increase rate). The correlation coefficient between -OH quantity and FE CO is as high as 0.98. Further study indicated that the presence of -OH can lead to a more compact electrochemical double layer (EDL) and charge transfer resistance by proton transfer. The -OH can also enhance CO 2 adsorption and stabilize the intermediate species (*COOH). DFT results further demonstrate that the rate-determining step was proton transfer from the surface -OH to MEACOO − , -OH modification can reduce the energy barrier to as low as 0.39 eV. This work provides additional insights into improving selectivity in amine-based cCO 2 RR, advancing the development of ICCU technology.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9
You-yun Gong,Xuejing Zhang,Jin-ping Cheng
Metal–organic frameworks (MOFs) offer tunable porosity and chemistry for advancing CO 2 capture. In this work, a ‘thermal-annealing–amine vapor deposition' strategy is proposed to synergistically engineer structural defects and uniformly distributed amine functionalities in UiO-66. Controlled annealing generates defect-rich UiO-66 (UiO-66-D) with exposed Zr 6 clusters, while subsequent hydrazine vapor deposition anchors amine groups directly at defective Zr nodes. The optimized material, N 2 H 4 @UiO-66-D, exhibits a markedly increased surface area (1449.36 m 2 /g) and achieves a CO 2 adsorption capacity of 2.60 mmol/g (at 298 K, 1 bar and pure CO 2 )—significantly higher than pristine UiO-66 (1.44 mmol/g at 298 K, 1 bar and pure CO 2 ). Enhanced CO 2 /N 2 separation performance is observed under simulated flue-gas conditions (at 1 bar, 298 K and 15 % CO 2 /85 % N 2 ), with IAST selectivity in the range of 111–33. Cyclic adsorption–desorption tests show no obvious decay in CO 2 uptake after ten cycles. Molecular dynamics (MD) simulations reveal that hydrazine modification increases free volume near defect sites, enhancing local CO 2 density. Density functional theory (DFT) calculations show that CO 2 preferentially adopts a bidentate surface adsorption (‘face-on') configuration at hydrazine-modified Zr defects, with an adsorption energy of −0.33 eV, confirming strong CO 2 activation and favorable binding. This work establishes a mechanistic framework for coupling defect engineering with vapor-phase amine functionalization, providing transferable design principles for the development of MOF-based CO 2 adsorbents.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Siyuan Huang,Xia Wang,Jia Liu,Bilyu Hong,Kai Yuan,Youzhu Yuan
Catalytic conversion of CO 2 to light aromatics (including benzene, toluene, and xylene, collectively known as BTX) and olefins is an eco-friendly approach for reducing waste gas emissions, but it remains a significant challenge. Traditional methods that modify the surface acid sites of zeolites to increase BTX selectivity often produce undesired byproducts and involve complex preparation processes. Here, we report a strategy to enhance BTX formation by altering the reaction intermediates using a tandem catalyst composed of metal oxides and dual-zeolite (GaZrO x /SAPO-34/ZSM-5, labelled as GZO/S34/Z5). The inclusion of S34 zeolite facilitates the partial transformation of CO 2 hydrogenation intermediates produced by GZO into light olefins, thereby promoting the aromatic formation in Z5. This results in a 72.6 % selectivity for total aromatics in hydrocarbons, with BTX accounting for a significantly higher selectivity compared to GZO/Z5, representing a 3.4-fold increase from 7.1 % to 24 %. Additionally, by regulating the acid density of Z5, the tandem catalyst with dual-zeolite can directly convert CO 2 and H 2 to 53.5 % aromatics and 25.5 % olefins, with a BTX selectivity of 13.8 % in hydrocarbons. This tandem catalyst design, through adjusting the reaction intermediates, offers an efficient method to inhibit the formation of light paraffin byproducts and enhance BTX selectivity in CO 2 conversion.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Rui Zhai,Haoliang Liu,Mengyue Gu,Zhuorui Wen,Bo Zhang,Jia Liu,Yonghong Cheng,Zhenyu Wang,Shaobin Wang,Jinying Zhang
The photocatalytic CO 2 reduction (CO 2 RR) to high-value-added chemicals such as ethylene (C 2 H 4 ) is desirable but challenging, due to the easy desorption of C 1 intermediates and insufficient C C coupling to C 2 intermediates. The CO 2 RR performance of violet phosphorus (VP) could be significantly altered by its electronic configurations, especially for C 2 H 4 selectivity. Herein, the effective electronic localization engineering of VP has been achieved by a well spatially dispersed dual-cocatalyst modification (VP-PA-Co₂P-Ag). The well distributed Co 2 P nanoflocs modification on VP were realized by prefunctionalization treatment of VP with phytic acid (PA). The metallic Co₂P and Ag were found to serve as bipolar system to induce more efficient surface electronic localization of VP and electronic enrichment on Co sites. The adsorption and activation of CO 2 , absorption and coupling of intermediates (CO ⁎ , CHO ⁎ ), and separation dynamics of photogenerated carriers have been demonstrated to be enhanced due to the significant orbital hybridization between CO 2 and Co 3d , which owing to the electronic localization on Co sites. Therefore, the C C coupling activity and selectivity on VP-PA-Co₂P-Ag has been demonstrated to be enhanced significantly to achieve 14.6 μmol g −1 h −1 and 69.9% electron selectivity of C 2 H 4 without any hole-sacrificial agent. The selective photocatalytic CO 2 -to-C 2 H 4 mechanism has been explored by in-situ diffuse reflectance infrared Fourier-transform, in-situ X-ray photoelectron spectroscopy, femtosecond ultrafast transient absorption, density of states, and Gibbs free-energy profiles, where the CO ⁎ intermediates could be easily adsorbed for protonation (CHO ⁎ ) and further C C coupling (COCHO ⁎ ), continuously reduced by successive proton-coupled multielectron transfer process to yield C 2 H 4 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Tianle Zhang,Changqing Chu,Wenjuan Bai,Yan He
CO 2 -assisted oxidative dehydrogenation of propane (CO 2 –ODHP) is a promising route to overcome the thermodynamic limitations of conventional propane dehydrogenation while enabling CO 2 utilization. However, PtSn/SiO 2 catalysts still suffer from rapid deactivation under CO 2 –ODHP conditions, the origin of which remains poorly understood. Herein, we systematically elucidate the deactivation mechanism of PtSn/SiO 2 catalysts and propose a silica encapsulation strategy to simultaneously suppress metal sintering and refractory coke formation. Although the introduction of CO 2 significantly reduces overall coke deposition, the PtSn/SiO 2 catalyst exhibits accelerated deactivation due to severe nanoparticle sintering and the accumulation of highly graphitized carbon species. By applying a controlled SiO 2 overcoating via a modified Stöber method, PtSn nanoparticles are effectively stabilized through the formation of robust Sn–O–Si anchoring linkages. An optimal silica loading of 5 wt% affords the Si(5)@PtSn/SiO 2 catalyst with a dramatically reduced deactivation rate constant (0.007 h⁻¹), while maintaining high propylene selectivity. Comprehensive TGA, Raman, and GC–MS analyses reveal that long-chain organosilane species (C 29 H 62 O 2 Si) constitute the key precursor for soluble coke species associated with silanol sites under CO 2 –ODHP conditions. The formation of these species is strongly correlated with the density of isolated surface silanol groups, which promote Si–O–C bond formation and permanently anchor coke precursors on the catalyst surface. The silica overcoating effectively modulates isolated silanol environment via enhanced hydroxyl condensation, thereby suppressing the generation of organosilane-derived coke nuclei. This work provides molecular-level insight into coke evolution on silica-supported Pt catalysts and demonstrates that balancing metal confinement with surface hydroxyl chemistry is critical for designing durable Pt-based catalysts for CO 2 -assisted propane dehydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
IEEE TRANSACTIONS ON ELECTRON DEVICES
·
2026
·
IF 3.6
Zifan Li,Jiazheng Liu,Songquan Yang,Mingchao Yang,Chuanyu Han,Xin Li,Li Geng,Yubin Yuan,Weihua Liu
Atomic layer deposition (ALD) has emerged as an important technique for dielectric fabrication in single-walled carbon nanotube field-effect transistors (SWCNT FETs). Notably, intrinsic SWCNTs are chemically inert and lack sufficient nucleation sites for the ALD process, which limits both the minimum thickness and interface quality of the dielectric layer. In this work, a pretreatment of SWCNTs with supercritical CO2 (SCCO2) fluids is introduced before ALD to improve the deposition quality. The SCCO2 pretreatment SWCNTs (SC-SWCNTs) demonstrate an increased number of nucleation sites on the surface for ALD dielectric fabrication, thereby improving the quality of the deposited gate dielectric layer and effectively reducing the interface state density. The experimental results reveal that the SCCO2-pretreatment SWCNT FET (SC-SWCNT FET) has an enhanced breakdown voltage of the dielectric layer and a reduction in interface state density, accompanied by a two-order-of-magnitude enhancement in the current on/off ratio. The SCCO2 treatment demonstrates superior dielectric-SWCNTs interface modification capabilities, establishing a viable pathway for developing high-performance SWCNT FETs for next-generation nanoelectronics applications.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yingtong Pan,Ruofan Li,Ling Zhang,Ji-Xuan Liu,Wenzhong Wang,Guo-Jun Zhang
Efficient conversion of dilute CO 2 into valuable products remains a significant challenge due to the low CO 2 concentrations (5–10%) in industrial flue gases, which are accompanied by inert gases and impurities. This results in low partial pressures, limited mass transfer, and dominant side reactions, undermining the efficiency and selectivity of CO 2 reduction reactions (CO 2 RR). To address this, we present a synergistic mechanochemistry–facet engineering strategy for efficient and selective CO 2 RR under ambient conditions using diluted CO 2 streams. By combining ultrasonic cavitation with mechanical stirring and exposing Cu 2 O (111) facets, the system achieves a CO yield of 1865.6 µmol g cat –1 , CO selectivity of 96.4%, and CO 2 conversion efficiency of 13.9% within one hour. These results surpass most previously reported systems for CO 2 reduction using low-concentration CO 2 streams. Mechanochemical activation enhances mass transfer and accelerates reaction kinetics, while facet engineering optimizes CO 2 adsorption and facilitates intermediate conversion. Density functional theory (DFT) calculations further reveal facet-dependent adsorption configurations and mechanochemical CO 2 RR pathways, clarifying the origins of the improved activity and selectivity. This approach provides a scalable solution for CO 2 conversion in low-concentration CO 2 environments, holding practical value in advancing industrial flue gas treatment and carbon capture and utilization (CCU) technologies.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2026
·
IF 4.3
Chuang Yue,Qian Su,Yi Li,Ying Liu,Yifan Liu,Yunong Li,Zifeng Yang
In this work, a novel graphene-reinforced polyimidazole microsphere catalyst with dual functionality for both CO 2 adsorption and epoxide activation was successfully synthesized via one-step suspension polymerization strategy. This heterogeneous catalyst contained no halogens, effectively mitigating environmental pollution, equipment corrosion, and ensuring product quality. Specifically, graphene was strategically incorporated into the catalyst matrix during synthesis to enhance its thermal stability, and the thermal decomposition temperature has increased by 23 °C. Under optimized reaction conditions, the catalysts with high nitrogen content ( e.g. G-NCHSM-1) achieved the highest yield of cyclic carbonate (99 %) from the cycloaddition of epoxide and CO 2 . Notably, the graphene-reinforced polyimidazole catalyst exhibited favorable stability and potential for industrial applications. Finally, based on the experimental characterizations and density functional theory (DFT) calculations, a possible mechanism for the synthetic cyclic carbonate was proposed, elucidating the synergistic effect of the imine group and C β -H on the imidazole ring in catalyzing the synthesis of cyclic carbonates from CO 2 . Therein, the imine group could capture CO 2 and activate epoxides.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Yanan Li,Jiangnan Yu,Yu Jiang,Yang Liu,Jun Wang,Minxia Wang,Zhaomin Li,Xueqin Li
A dual transport channels network constructed within mixed matrix membranes (MMMs) has revealed the potential to enhance separation performance. In this study, Cu-TCPP(BA) nanosheets with unsaturated copper sites were synthesized as suitable fillers. Subsequently, Cu-TCPP(BA) nanosheets were incorporated into Pebax® MH 1657 (Pebax) to fabricate MMMs for CO 2 separation. Cu-TCPP(BA) nanosheets significantly enhance CO 2 /CH 4 separation performance by constructing dual transport pathways within the mixed matrix membrane. This mechanism centers on the dual pathways: on one hand, gas molecules can diffuse through the intrinsic microporous channels of the nanosheets; on the other hand, they can also be transported via the interlayer channels formed by the stacking of nanosheets. The synergistic effect of these two pathways collectively enhances the efficient permeation and selective sieving of CO 2 . Furthermore, the regularly aligned unsaturated copper sites on the nanosheet surface act as strong Lewis's acid active centers, preferentially adsorbing CO 2 molecules through quadrupole moment interactions, which provides the chemical basis for high separation selectivity. The adsorbed CO 2 then rapidly diffuses along the dual pathways, forming an “adsorption-diffusion” synergistic transport network. In comparison to pure Pebax membranes, the mixed matrix membranes (MMMs) infused with 3 wt% Cu-TCPP(BA) demonstrated excellent CO 2 separation performance, exhibiting a 77% enhancement in CO 2 permeability and a 44% improvement in CO 2 /CH 4 selectivity. The use of 2D fillers to create a dual transport channels network is an efficiency approach for enhancing CO 2 separation in MMMs.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）