Small
·
2023
·Vol. 19
·期 45
·2302683
·
IF 13.3
Bixia Yang,Xingpeng Jiang,Yanting Zheng,Linxin Zhou,Jiawei Yan,Zanyong Zhuang,Yan Yu
Orderly heterostructured catalysts, which integrate nanomaterials of complementary structures and dimensions into single-entity structures, have hold great promise for sustainability applications. In this work, it is showcased that air as green reagent can trigger in situ localized phase transformation and transform the metal carbonate hydroxide nanowires into ordered heterostructured catalyst. In single-crystal nanowire heterostructure, the in situ generated and nanosized Co 3 O 4 will be anchored in single-crystal Co 6 (CO 3 ) 2 (OH) 8 nanowires spontaneously, triggered by the lattice matching between the (220) plane of Co 3 O 4 and the (001) plane of Co 6 (CO 3 ) 2 (OH) 8 . The lattice matching allows intimate contact at heterointerface with well-defined orientation and strong interfacial coupling, and thus significantly expedites the transfer of photogenerated electrons from tiny Co 3 O 4 to catalytically active Co 6 (CO 3 ) 2 (OH) 8 in single-crystal nanowire, which elevates the catalytic efficiency of metal carbonate catalyst in the CO 2 reduction reaction ( V CO = 19.46 mmol g −1 h −1 and V H2 = 11.53 mmol g −1 h −1 ). The present findings add to the growing body of knowledge on exploiting Earth-abundant metal-carbonate catalysts, and demonstrate the utility of localized phase transformation in constructing advanced catalysts for energy and environmental sustainability applications.
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ENERGY & FUELS
·
2023
·
IF 5.3
Junhui Liu,Bing Li,Mengting Li,Yuan Hu,Shan Han,Xinwen Guo
Transformation of abundant and economical feedstock CO2 and renewable H2 into valuable hydrocarbons is considered a prospective route for the storage of renewable energy. However, it is also a challenge to prepare highly stable and active catalysts. Herein, active and stable catalysts were designed by pyrolysis of the Fe-modified bimetal-ZIFs with varied ratios of Zn/Co, in order to introduce Zn in situ as a structure promoter and Co for an increase of the CO2 conversion. CO2 conversion increased by improving the Co content, while CH4 selectivity also increased obviously. The superior selectivity of value-added hydrocarbons and the ratio of olefins and paraffins (O/P) were obtained without addition of alkali metals. The O/P is 1.76 over FeZnCo-NC-59. The N-doped porous carbon catalysts delivered a good stability in a 1000 h test under harsh reaction conditions. The stable catalysts provide a promising prospect for further application in CO2 hydrogenation.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xiangyang Liu,Jianchun Chu,Shaoxuan Huang,An Li,Shuanlai Wang,Maogang He
Ionic liquids (ILs) are considered excellent substitutes for aqueous alkanolamine solutions in CO2 capture systems. However, the smart design of ILs, facing the small sparse data set and complex ionic structures, poses a huge challenge. To address this issue, a novel machine learning method based on a syntax-directed variational autoencoder (SDVAE), deep factorization machine (DeepFM), and gradient-based particle swarm optimization (GBPSO) was proposed in this work. The SDVAE converts the molecular structure and chemical space of the ILs, and then DeepFM predicts the solubility of each coordinate in the chemical space representing an IL. Finally, GBPSO identifies the coordinates that represent ILs with ideal properties. Our main optimization objective is a high solubility difference for CO2 between its absorption and desorption conditions in commercial plant capture systems, which represents the CO2 capture ability. The best IL generated has a predicted solubility difference that is 35.3% higher than that of the best one in the data set. A synthetic novel IL [EMIM][TOS] from the generated results was experimentally evaluated; it has a sufficiently high solubility difference to be a capture solvent with low energy consumption. Our model has proved to be a high-efficiency molecular design model that can be used for sparse small data sets.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ge Yang,Yanjiao Wang,Mengling Sun,Panpan Xu,Chunzheng Wang,Ke Huang,Heqing Jiang,Svetlana Mintova,Hailing Guo
The amino-modification of the filler material is one of the most common strategies for optimization of the performance of mixed matrix membranes, aiming to enhance the interactions between the filler and the organic matrix and accelerate the adsorption of gas molecules by the filler. Herein, we found that the in-situ introduction of amino groups into the HKUST-1 filler would have negative effects on the gas separation performance of the MMMs following the “diffusion-adsorption coupling control” mechanism, which suggests that using MOFs fillers with large aperture size to accelerate the diffusion of small H 2 molecules and slow the diffusion of polar CO 2 molecules through the adsorption-desorption process. The NH 2 -HKUST-1 filler caused the blockage and loss of the pore structure , and the interfacial interactions in the PEI-based mixed matrix membranes were not improved. Therefore, the in-situ synthesized NH 2 -HKUST-1 did not support H 2 /CO 2 separation. This work further investigates the possible “diffusion-adsorption coupling control” mechanism of fillers with large aperture size and contributes to the development of MMMs materials.
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ENERGY & FUELS
·
2023
·
IF 5.3
Yi Ren,Yujia Bai,Genxiang Wang,Yijian Liu,Chuancheng Mou,Jiayu Chen,Baohuan Wei,Hui Wang,Yuhan Sun
Efficient conversion of CO2 to value-added fuels or chemicals using electricity from renewable sources is an appealing approach to realize carbon neutrality. Under this background, it is crucial to design efficient and low-cost catalysts for CO2 electroreduction. Herein, we fabricated an electrocatalyst with the structure of Cu–Ni alloy nanoparticles grown on nitrogen-doped carbon nanotubes (CuxNi/NCNT, x = 2.4, 1, and 0.36) for electrochemical CO2 reduction reaction (CO2RR) via a hydrothermal method followed by pyrolysis. The optimized CuNi/NCNT demonstrates a favorable CO2RR performance with a CO Faradaic efficiency (FECO) of 94.8% and a current density of 26.6 mA cm–2 at −0.9 V versus the reversible hydrogen electrode (vs RHE) in the H-cell, far superior to those of single metal counterparts. Density functional theory (DFT) calculations unravel that the Cu–Ni alloys possess much lower free energy changes for the formation of the key COOH* intermediate than those of the Cu metal, thereby facilitating CO2 reduction into CO. Additionally, the CO2RR performance of CuNi/NCNT was further evaluated in the gas diffusion electrode (GDE) involved in the flow cell to examine the practical application of the prepared catalyst, which can deliver a current density of 124.6 mA cm–2 with a FECO of 92.8% at −1.1 V vs RHE. This work enriches electrocatalysts for highly efficient CO2 electroreduction to CO.
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ChemCatChem
·
2023
·Vol. 15
·期 15
·e202300440
·
IF 4.5
Xiaoyue Zhang,Yong Yang,Lijun Xiong,Tianyu Wang,Mengwei Xue,Jianhua Ge,Zheng Tang,Panjie Li,Nan Yin,Jinyou Shen
Graphical Under light excitation , WOS broadens the photo-response range through Z-scheme heterojunction. Its photothermal effect can convert light into heat and accelerate the reaction. This efficient photothermal technology facilitates CO 2 reduction. Photothermal CO 2 reduction using H 2 O combined with photocatalysis-driven H 2 O splitting combined with thermal catalysis-supported CO 2 reduction has attracted rapid interest in artificial synthesis of solar fuel. With respect to extremely efficient photothermal catalysis, the photothermal impact of TMDCs (Transition Metal Dichalcogenides) facilitates CO 2 reduction by activating lattice oxygen in oxide to enhance H 2 O oxidation. However, the fixed band gap of single photocatalyst is limited. The purpose of this work is to expand the band gap and improve the redox capacity. Hollow boxwood ball-like WO 3 /WS 2 Z-scheme heterojunctions were prepared and used for photothermal catalytic CO 2 reduction. DFT calculations and UV-Vis spectra show LSPR effect in WOS heterojunctions, and the optical response extends to near infrared region. By comparison, the photothermal catalytic reduction of WO 3 /WS 2 (9.717 μmol) by CO 2 at 513 K is higher than that at 298 K (1.198 μmol) by a factor of 8. The formation of Z-scheme heterojunction promotes rapid carrier transfer and lowers the reaction energy barrier. As well as the hollow structure improves light utilization and increases the interfacial area and number of active sites. In addition, the WO 3 /WS 2 heterostructure utilizes its unique LSPR effect to generate heat through the photothermal effect, which can also promote molecular activation. This work reveals the important role of the LSPR effect in photothermal catalysis and demonstrates a TMDCs-based photothermal-driven catalysts, which presents a promising approach for designing of photothermal catalytic CO 2 reduction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Haiying Xu,Zhaoliang Wang,Hehua Liao,Dongmiao Li,Jinni Shen,Jinlin Long,Wenxin Dai,Xuxu Wang,Zizhong Zhang
Photocatalytic converting CO 2 into C 2 products is highly desirable but is extremely sensitive to catalyst structure. In this work, Ti-H species and oxygen vacancies are simultaneously integrated on hydrogenated SrTiO 3 surface by thermally treating with NaBH 4 , which promotes the activation of CO 2 into HCOO - and CO* intermediates. The proximity of oxygen vacancies and Ti-H species contributes to the C-C coupling of intermediates into acetylene (C 2 H 2 ) products. To the best of our knowledge, this is the first example for the photocatalytic CO 2 reduction into C 2 H 2 main products. The optimal hydrogenated SrTiO 3 has the C 2 H 2 yield of 39.0 μmol·g −1 with a 76.0 % selectivity among C 2 products. Therefore, this work provides an approach of designing the adjacent active sites for photocatalytic CO 2 conversion into C 2+ products.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yajun Wei,Tan Zhao,Jiawei Wang,Yanli Chen,Qiang Wang,Xizheng Liu,Yunfeng Zhao
The development of an ultramicroporous (<7 Å) adsorbent with a narrow pore distribution for capturing and adsorbing gas molecules has received a lot of attention. In this paper, the commercial carbon molecular sieve (CMS) was used as the precursor, and a carbon molecular sieve (CMS-A-5) with better performance was obtained by activating with potassium hydroxide (KOH). After activation, the ultramicroporous volume increased from 0.163 cm3 g–1 (CMS) to 0.329 cm3 g–1 (CMS-A-5), and the CO2 capacity increased from 42.76 to 71.92 cm3 g–1 at 298 K and 1 bar. The breakthrough experiments demonstrated that the CO2 capture ability of CMS-A-5 increased by ∼9.5 times for the respiratory air containing CO2/O2/N2 (4:20:76) and was easily regenerated and reused. CMS-A-5 was also capable of selectively capturing VOC molecules including benzene, toluene, and C8 alkyl aromatics (BTEX) with a high adsorption capacity at a low pressure. The excellent CO2 and VOC molecule adsorption capacity make CMS-A-5 a promising candidate for selective separation of the gas mixture, in particular, for air purification in confined spaces.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Tongxin Liu,Ruili Zhang,Guangcan Huang,Yabo Xie,Lin-Hua Xie,Jian-Rong Li
Emerging as a new type of porous materials, metal-organic cages (MOCs) show great potential in adsorption and separation. The high porosity and solubility of MOCs have generated increasing interest in their use as fillers for preparing mixed matrix membranes (MMMs). Herein, we present a series of zirconocene-based MOCs (MOC-1, MOC-1-NH 2 , and MOC-1-4F), which were used to fabricate MMMs with polyimide 6FDA-DAM. Particularly, the perfluorinated MOC (MOC-1-4F) could form a clear casting solution with 6FDA-DAM in some solvents. The resultant MMMs were analyzed by AFM, SEM, EDX-mapping, XRD, CSM, Raman, TG, and DSC measurements, indicating that MOC-1-4F were homogeneously dispersed in 6FDA-DAM, and the T g values, mechanical property, CO 2 solubility and diffusivity of the membrane were promoted after the introduction of MOC-1-4F. The MOC-1-4F based membranes also outperformed the membranes with MOC-1 or MOC-1-NH 2 as filler in CO 2 /CH 4 separation. A low MOC-1-4F loaded MMM (MOC-1-4F-2.17%) exhibited 57% improved CO 2 permeability (1228 barrer) in comparison with 6FDA-DAM membrane, and the CO 2 /CH 4 selectivity reached 22, surpassing the 2008 Robeson upper-bound. The plasticization effect was significantly alleviated in MOC-1-4F-2.17%, indicating that the MOC-1-4F-2.17% is potential for CO 2 /CH 4 separation. This work demonstrates that the gas separation performance of MOC-based MMMs could be fine-tuned by the structural tailoring of MOCs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Meidan Que,Weihua Cai,Yang Zhao,Yawei Yang,Boyue Zhang,Sining Yun,Jin Chen,Gangqiang Zhu
Mimicking the natural photosynthesis process to convert carbon dioxide into value-added chemicals is vital to solving both the climate crisis worldwide and the depletion of fossil fuels. Herein, we explore the synthesis of 2D FAPbBr 3 nanoplate combined with 2D Ti 3 C 2 nanosheet to form a 2D/2D FAPbBr 3 /Ti 3 C 2 Schottky heterojunction using facile hot-injection and in-situ growth approaches. The Schottky heterojunction of FAPbBr 3 /Ti 3 C 2 over large interfacial contact provides abundant channels for transferring photogenerated carriers from FAPbBr 3 nanoplate to Ti 3 C 2 nanosheet. The experimental results showed a CO yield of 93.82 μmol·g −1 ·h −1 with ethyl acetate/deionization water as a sacrificial reagent for FAPbBr 3 /Ti 3 C 2 composite, which was 1.25-fold enhancement that on pristine FAPbBr 3 nanoplates. The large 2D heterointerface can efficiently accelerate the spatial separation and transfer of photogenerated carriers and result in the superior photocatalytic activity and favorable stability of FAPbBr 3 /Ti 3 C 2 photocatalysts, which are proved by in-situ X-ray photoelectron spectroscopy, photoluminescence, transient absorption spectra, and Mott-Schottky measurement. Thus, this work unveils that 2D/2D Schottky heterostructures would significantly improve the reaction activities of halide perovskite-based photocatalysts.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Da Wang,Ying Zhu,Weiting Yu,Zhiqiao He,Feilong Dong,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Lizhang Wang,Shuang Song
Ag-based electrodes have emerged as important candidates for the industrial electrochemical CO 2 reduction reaction (eCO 2 RR) to form CO. Herein, an intrinsic versatile Ag electrode has been derived in situ from Ag-MOF on Ag foam (denoted as ER-AF), which exhibits the highest current density (57.2 mA cm −2 ) at a potential of −1.15 V vs. RHE reported to date for the formation of CO in a commonly used H-type cell. ER-AF has multiple-roles: The 3D dendrite structure promotes mass diffusion; the rich edges sites favor CO 2 adsorption and conversion, and the highly exposed (111) facet facilitates the desorption of CO. Their cooperating functions result in the remarkable performance of ER-AF in the eCO 2 RR to form CO. This work offers an effective strategy to achieve high eCO 2 RR activity and selectivity by assembling the active and stable sites together on the MOF-derived materials.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Shuoyu Wang,Xianyu Qiu,Yangguan Chen,Shuixia Chen
Amine-functionalized porous adsorbent is one kind of important materials in carbon dioxide capture due to its stability and efficiency. In this study, a copolymer (polyHIPE) with interconnected macropore networks, hierarchical porous structure and abundant branched amino groups was prepared by high internal phase emulsion (HIPE) strategy via copolymerization of styrene (St), divinylbenzene (DVB), tetraethyl orthosilicate (TEOS), and triethoxyvinylsilane (VTEO), and then a novel amine-functionalized CO 2 adsorbent was synthesized by in situ ring-opening grafting copolymerization of aziridine with the polyHIPE. The structure, morphology, and physicochemical properties of the polyHIPEs were characterized by FTIR, TEM, TGA , and SEM. The key roles of VTEO and TEOS in introducing active hydroxyl groups onto the surface of the inert polymer was evaluated, which was essential to improve the hydrophilicity of the polyHIPE and to provide reactive sites to combine with amine agents. The contact angle of the polyHIPE while copolymerized with TEOS and VTEO significantly was decreased from 144° to 72°. In order to further increase the specific surface area of the polyHIPEs, post crosslinking of polyHIPEs was implemented through a Friedel–Crafts reaction. The specific surface area of post-crosslinked polyHIPE could reach 513 m 2 /g, which was proven to be effective to enhance its CO 2 adsorption capacity. Finally, the abundant branched amino sites via aziridine grafting and high surface area greatly enhanced CO 2 adsorption capacity of the amino-modified polyHIPEs. The adsorption capacity of 2.40 and 3.25 mmol CO 2 /g could be achieved under dry and humid conditions in 0.1 atm partial pressure of CO 2 , respectively.
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