ChemCatChem
·
2017
·Vol. 10
·期 6
·1272-1276
·
IF 4.803
Yulong Zhang,Donglong Fu,Xianglin Liu,Zhengpai Zhang,Chao Zhang,Bianfang Shi,Jing Xu,Yi-Fan Han
Understanding of dynamic structure of active sites is of paramount importance for rational design of industrial catalysts. This work revealed the structure evolution of iron active phases for CO 2 hydrogenation over iron-based catalysts. With a combination of operando Raman spectroscopy and X-ray Diffraction coupled with online gas chromatography, the panoramic structure evolution of iron oxides (α-Fe 2 O 3 and γ-Fe 2 O 3 ) during activation and CO 2 hydrogenation were elaborated, that is, α-Fe 2 O 3 (γ-Fe 2 O 3 )→α-Fe 3 O 4 (γ-Fe 3 O 4 )→α-Fe (γ-Fe)→χ-Fe 5 C 2 (θ-Fe 3 C). Both iron carbides showed high catalytic activities while χ-Fe 5 C 2 exhibited higher selectivity to lower olefins but weaker chain growth probability than θ-Fe 3 C. Graphical Using operando techniques including Raman spectroscopy (ORS)-gas chromatography (GC) and operando X-ray diffraction (OXRD)-GC, we demonstrated that χ-Fe 5 C 2 and θ-Fe 3 C driven from α-Fe 2 O 3 and γ-Fe 2 O 3 precursors, respectively, are the active phases that are responsible for the different distribution of products.
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RSC Advances
·
2018
·Vol. 8
·期 62
·35521-35527
·
IF 2.936
Xia Wang,Wulan Zeng,Qingjie Guo,Qijin Geng,Yongmei Yan,Xiude Hu
To systematically study CO2 adsorption performance, semicoke from the low-rank lignite was further activated and functionalized for CO2 capture from flue gases. The effect of the activation conditions, such as the activation temperature, activation time and HCl washing, and the tetraethylenepentamine (TEPA)-functionalization on CO2 adsorption were investigated; the pore structure and surface morphology of the semicoke under different activation conditions were characterized. Both the surface structure and adsorption performance of the activated semicoke could be improved under appropriate activation and acid-treatment conditions. The optimal breakthrough and equilibrium adsorption capacity for the TEPA-functionalized HCl-washed activated semicoke were separately 2.68 and 3.70 mmol g−1 at 60 °C for the simulated flue gas of 15 vol% CO2 and 85 vol% N2. After ten adsorption–desorption cycles, the equilibrium adsorption capacity was still 3.43 mmol g−1, and the semicoke-based sorbent showed good regenerability.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 6
·1504-1511
·
IF 2.726
He Kai,Liu Shijia,Zhao Guiyan,Qin Yucai,Bi Yanfeng,Song Lijuan
A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(Ni x W/SBA-15, Ni-5%, x =1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), transmission electronic microscopy(TEM), H 2 -temperature programmed reduction(H 2 -TPR), and X-ray photoelectron spectroscopy(XPS). High-resolution TEM images, XPS measurements, H 2 -TPR experiments coupled with PXRD results determined the evolution of Ni and W species. It is found that a trace amount of W from H 2 WO 4 can significantly improve Ni dispersion on SBA-15 (Ni 50 W/SBA-15) with Ni 0 and non-stoichiometric WO x species as small as ca . 3.6 nm. The prepared Ni x W/SBA-15 was utilized for CO 2 hydrogenation, which showed that a higher W content restrained the CO 2 hydrogenation while a lower W ratio promoted both conversion rate and selectivity for methane compared with Ni/SBA-15. The Ni 50 W/SBA-15 catalyst showed the best performance with a 93.3% CO 2 conversion rate and 99.7% selectivity for methane at 400 o C under 0.1 MPa and maintained ca . 97% initial performance for 24 h. Tracking product evolution experiments by in-situ Fourier transform infrared spectrascopy(FTIR) indicated that a small amount of W can modify the surface of Ni particles by geometric coverage and electronic modification, which facilitates the adsorption of the CO intermedia and results in the formation of CH 4 . This work provides a new clue to fabricating efficient CO 2 conversion bimetallic materials.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Qingru Yang,Qinghong Shi,Xiaoyan Dong,Linling Yu,Yan Sun
Hydrolysis of organophosphates (OPs) with organophosphate hydrolase (OPH) provides a green approach to degrading OPs, but the success of enzymatic OPs degradation relies on the availability of high-efficiency OPH. Herein, we report a simple but effective way to constructing high-performance OPH preparations based on the in situ encapsulation of hexahistidine-tagged OPH (H 6 -OPH) into cobaltous zeolitic imidazolate framework (ZIF-67) via biomineralization. ZIF-8 made of the same organic ligand but a different metal ion (Zn 2+ ) was used for comparison. It was found that the H 6 -tag domain did not affect the catalytic properties of OPH in the absence of Co 2+ , but boosted the Co 2+ -activation effect on the H 6 -OPH catalytic activity by two-fold. Furthermore, H 6 -OPH@ZIF-67 retained the highly boosted activity, while H 6 -OPH@ZIF-8 and OPH@ZIF-67/ZIF-8 lost most of the activities. Extensive analysis revealed that the H 6 -tag promoted the Co 2+ -induced OPH conformation transition and locked the activated conformation in ZIF-67. Notably, H 6 -OPH@ZIF-67 not only achieved an activity recovery as high as 348 % and a 321 % increased catalytic efficiency ( k cat / K m ) over free OPH, but also exhibited greatly improved stability and reusability. The findings underscore the high efficiency of fabricating high-performance OPH preparations via polyhistidine-tag fusion, Co 2+ activation and locking by the cobalt-organic framework.
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PubMed
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Jiage Yu,Wei Liu,Lu Bai,Benqiang Tian,Qingyi Zhu,Qianxi Yang,Linlin Zhou,Haoyang Wu,Yuan Wang,Boyuan Li,Xiangrong Jin,Yun Kuang,Jiazhan Li,Xiaoming Sun
CO 2 electroreduction typically requires large overpotentials to sustain high reaction rates, which at current densities approaching 1 A cm −2 inevitably intensify competition from the hydrogen evolution reaction (HER), making it difficult to simultaneously sustain high product selectivity (>95%). In this study, hollow Ni─NC (H-Ni-NC) was synthesized using nanoscale silica sphere templates and atomic Zn as a sacrificial pore-former within the carbon shell. The optimized H-Ni-NC achieves a current density of −1.0 A cm −2 with over 95% CO Faradaic efficiency in a flow cell. The high performance was attributed to the hollow sphere architecture enriched with gas-permeable through-pores. Notably, the Zn dosage selectively modulates the shell through-porosity, without altering hollow sphere macrostructure or the active-site structure, thereby enabling a systematic investigation of porosity effects. Finite-element simulations provide a qualitative framework suggesting a trade-off between reactant transport and active surface area with increasing porosity in hollow spherical catalysts. This work underscores that engineering of the nanoscale mass-transport environment surrounding active sites plays a critical role in designing high-efficiency electrocatalysts.
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PubMed
高影响因子
Nanomaterials
·
2026
·Vol. 16
·期 14
·872
·
IF 4.8
Huiqing Dong,Siyu Huang,Haopeng Cui,Ziyi Zhang,Dongxu Zhou,Weikai Huang,Xiaodong Zhang,Zhongxiao Zhang,Jianqiu Lei,Ning Liu
The conversion of CO2into value-added chemicals using photothermal catalysis is an attractive approach for achieving carbon neutrality. However, the limited visible-light absorption and rapid charge carrier recombination of CeO2hinder its photothermal catalytic performance. Herein, a series of In2O3-modified CeO2(In2O3-CeO2) are fabricated from a Ce-BTC metal–organic framework (MOF) precursor and applied to photothermal CO2hydrogenation. This approach not only effectively modulates the pore structure but also generates abundant oxygen vacancies (Ov). As a result, CO2adsorption and activation, charge separation and photothermal catalytic performance over In2O3-CeO2are significantly enhanced. The 3% In2O3-CeO2(3% denotes amounts of In) composite catalyst exhibits the optimal catalytic performance with a CO yield of 92.35 mmol·g−1·h−1and a remarkable 100% selectivity. A mechanistic study reveals that the Ov-rich interface facilitates electron transfer and promotes CO2conversion through a CO2→ *COOH → *CO reaction pathway. This work provides an effective strategy for designing high-efficiency MOF-derived composites to achieve carbon utilization.
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高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2026
·
IF 6
Wang Haixia,Sun Yilei,Liu Chuang,Meng Zeda D.,Oh Won-Chun
A series of graphene-modified copper–metal–organic framework composites (G-Cu-MOF-0.3, G-Cu-MOF-0.5, G-Cu-MOF-1) were fabricated via a solvothermal method. Structural characterizations verified that graphene was successfully composited without damaging the Cu-MOF crystalline framework, among the four materials, G-Cu-MOF-0.5 exhibits the largest specific surface area and pore size. Electrochemical results showed that G-Cu-MOF-0.5 displayed the best CO₂ electroreduction performance, with a current density of − 11 mA cm⁻², a double-layer capacitance (Cdl) of 4.97 mF cm⁻² and a Tafel slope value of 36.5 mV dec⁻¹. At − 1.5 V vs. RHE, the total Faradaic efficiency for CH₄ and CO reached 24% with stable operation over 12 h. Graphene modification significantly improves the conductivity, active site density, and structural stability of Cu-MOF, realizing efficient and controllable CO 2 conversion to C1 products. The hydrogen evolution reaction (HER) remains the dominant side reaction, and the Faradaic efficiency toward CH 4 is still moderate, leaving room for further selectivity optimization.This work provides a feasible strategy for designing MOF–carbon composites for electrocatalytic CO₂ reduction to methane.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Shucheng Tian,He Tao,Zhifang He,Tingting Chang,Bin Li,Jianye Li,Xueqing Li,Lu Wang,Zibo Yang,Zhihua Qiao
Ti 3 C 2 T x is a two-dimensional sheet-like material with abundant and tunable surface functional groups, showing excellent gas adsorption and transport ability in CO 2 separation. However, it suffers from several intrinsic limitations, including susceptibility to oxidation, restacking, and humidity sensitivity, which prevent it from being used alone as a membrane material for complex application scenarios. In this work, meltable ZIF-62 was selected as the continuous phase and Ti 3 C 2 T x as the dispersed phase. Thermal treatment was used to promote the softening and flow of ZIF-62, enabling the embedding and immobilization of Ti 3 C 2 T x . Finally, self-supporting Ti 3 C 2 T x /a g ZIF-62 composite glass membranes were obtained, and their gas separation performance was evaluated. The results show that the introduction of Ti 3 C 2 T x effectively improves the CO 2 permeability of the composite membranes while maintaining high separation selectivity. Specifically, the best overall performance was achieved at a doping content of 1 wt%, where the CO 2 permeability increased from 1403 Barrer to 5124 Barrer, and the ideal CO 2 /N 2 and CO 2 /CH 4 selectivities reached 44.9 and 30.7, respectively. The CO 2 /N 2 separation performance of this membrane exceeds the latest upper bound, while its CO 2 /CH 4 separation performance also shows a competitive level. In addition, this membrane maintained relatively stable performance in humid-gas, pressure-variable, and 160 h continuous operation tests.
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ENERGY & FUELS
·
2026
·
IF 6
Jiayou Liao,Junling Lin,Shuangming Wang,Zhichao Zhai,Xianjie Meng,Yangyang Wang,Yong Wang,Chengyun Gao,Fanhui Meng,Jinping Li
Mixed matrix carbon molecular sieve membranes are gas separation membranes that combine the synergistic effects of carbon molecular sieves and inorganic components. The DD3R molecular sieve exhibits significant molecular size sieving effects and demonstrates high adsorption selectivity toward CO2. Against the backdrop of the current push for carbon neutrality, highly efficient CO2 separation materials are of great significance to the development of carbon capture and storage (CCS) technology. This is particularly true in natural gas purification and industrial exhaust gas treatment, where higher demands are placed on the efficient separation of CO2 and CH4. Based on this, this study used the DD3R molecular sieve as the functional filler, used 6FDA-DAM polyimide as the precursor, and obtained the hybrid matrix carbon membrane through a high-temperature carbonization process. The microstructure and physicochemical characteristics of the carbon membranes were systematically characterized using scanning electron microscopy and other techniques, and the effect of DD3R loading on their gas separation performance was investigated. The results indicate that as the doping concentration of DD3R molecular sieves increases, both the CO2 permeability and CO2/CH4 separation selectivity of the mixed matrix carbon molecular sieve membranes exhibit a trend of initially increasing and then decreasing. Furthermore, when the DD3R doping mass fraction reached 0.3 wt %, the prepared carbon membrane exhibited optimal performance, achieving a CO2 permeability coefficient of 29,679 Barrer and a CO2/CH4 selectivity of 33.1, surpassing the Robeson upper limit reported in 2019. The results indicate that, owing to the unique pore structure of the DD3R molecular sieve and its synergistic interaction with the carbon matrix, the carbon membrane effectively overcomes the trade-off between permeability and selectivity, demonstrating significant potential for industrial applications and holding broad prospects in the field of carbon capture.
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·
IF 6.7
Xianglong Li,Zhicong He,Haoxian Huang,Yachuan Yuan,Yanbin Feng,Wei Peng,Song Xue
2,4-Dihydroxybenzoic acid is an important intermediate in agricultural and food chemistry. Salicylic acid decarboxylase catalyzes the carboxylation of resorcinol with CO2 to yield 2,4-dihydroxybenzoic acid. However, this process suffers from poor regioselectivity and low carboxylation activity. Here, we propose that the unique microenvironment created by the enzyme’s substrate-binding pocket, referred to here as the enzyme field, induces charge redistribution in resorcinol, thus altering the enzymatic regioselectivity. Charge distributions at carbon atoms were calculated under 14 different enzyme fields, and catalytic assays revealed the correlation between regioselectivity and the electronegativity of the corresponding carbon atom. Furthermore, K23A/Y64T/E291D/Y27A was obtained with 99% C4-carboxylation selectivity from 20%, and a 69-fold increase in kcat/Km. The SAD-catalyzed carboxylation mechanism involving HCO3–-mediated proton transfer was proposed on the basis of QM/MM metadynamics simulations. This work elucidates the repurposing of regioselectivity by enzyme-induced substrate charge distribution and proposes the mechanism of the SAD-catalyzed carboxylation of resorcinol.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Yu-Jiao Li,Qi-Qi Huang,Shi-Chao Qi,Xiao-Qin Liu,Lin-Bing Sun
CO2 adsorption is a key technology for carbon capture. Current applications primarily focus on large-scale industrial CO2 emission sources, while the capture from distributed sources, especially kitchen flue gas, has been ignored. The kitchen flue gas is featured by low CO2 concentrations, high humidity, and high concentrations of volatile organic compounds. Such a complex composition leads to competitive gas adsorption and rapid degradation of the adsorbent performance. Herein, to solve this problem, xP/D-carrier adsorbents are synthesized by coloading polyethylenimine and diethanolamine onto the three SiO2 carriers (fumed silica, hierarchically porous SBA-15, and mesostructured KIT-6). Among them, 0.9P/D-KIT-6 performs the best chemical CO2 adsorption capacity of 2.22 mmol/g at 348 K and 1.0% (vol.) CO2 concentration, showing excellent thermal stability and ultrahigh CO2/N2 selectivity of 1030. Breakthrough tests with simulated kitchen flue gas show that xP/D-carrier adsorbents maintain high CO2 adsorption selectivity under elevated temperatures and complex gas environments.
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Catalysts
·
2026
·Vol. 16
·期 8
·725
·
IF 4.5
Hongtao Xie,Limi Yan,Shijian Lu,Pengcheng Xiang,Dongliang Liu,Lili Wang
The electrocatalytic reduction of CO2into value-added chemicals offers a promising route to mitigate greenhouse gas emissions, yet the uncontrollable structural reconstruction and surface rearrangement of electrocatalysts during operation often lead to severe activity degradation. Herein, we reveal that Bi2O2SO4(BSO) undergoes an irreversible phase transformation into Bi2O2CO3(BCO) nanosheets accompanied by the partial reduction of Bi3+to metallic Bi0under cathodic potentials. A series of BCO/BSO heterojunction catalysts with tunable compositions are synthesized via a mild in situ ion-exchange method. To circumvent the detrimental effects of this dynamic reconstruction, we devise a pre-activation strategy that deliberately completes the structural evolution prior to electrocatalysis. The optimized 20%-BCO/BSO heterojunction achieves a remarkable Faradaic efficiency of 98.4% for formate production in a flow cell at elevated potentials, with >95% FE(HCOOH)over a wide potential window (−0.8 to −1.7 V vs. RHE). In situ infrared spectroscopy elucidates that the reconstructed interface can promote CO2adsorption, stabilize the *OCHO intermediate, and facilitate HCOOH desorption. This work provides experimental evidence of the reconstruction behaviour of bismuth-based catalysts and offers a rational design method for constructing structurally stable heterojunction electrocatalysts.
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