INORGANIC CHEMISTRY
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2022
·
IF 5.436
Yimeng Zhou,Qianjin Ye,Xiangli Shi,Qiong Zhang,Qi Song,Changjian Zhou,Di Li,Deli Jiang
Due to the multiple electron and proton transfer processes involved, the photogenerated charges are easily recombined during the photocatalytic reduction of CO2, making the generation of the eight-electron product CH4 kinetically more difficult. Herein, Ni3B nanoparticles modulated by p-block element were combined with TiO2 nanosheets to construct a novel Schottky junction photocatalyst (Ni3B/TiO2) for the selective photocatalytic conversion of CO2 to CH4. The formed Ni3B/TiO2 photocatalyst with Schottky junction ensures a transfer pathway of photogenerated electrons from TiO2 to Ni3B, which facilitates the accumulation of electrons on the surface of Ni3B and subsequently improves the activity of photocatalytic CO2 reduction to CH4. The optimized Ni3B/TiO2 Schottky junction shows an improved CH4 yield of 30.03 μmol g–1 h–1, which was much higher than those of TiO2 (1.62 μmol g–1 h–1), NiO/TiO2 (2.44 μmol g–1 h–1), and Ni/TiO2 (4.3 μmol g–1 h–1). This work demonstrated that the introduction of p-block elements can alleviate the scaling relationship effect of pure metal cocatalysts to a certain extent, and the modified Ni3B can be used as a promising new cocatalyst to effectively improve the selective photocatalytic of CO2 to CH4.
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高影响因子
Nano Research
·
2022
·Vol. 16
·期 4
·4786-4792
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IF 10.269
Zhang Jin,Gao Mengting,Wang Ruiyi,Li Xincheng,Huang Tianfen,Wang Jing,Wang Yunwei,Zheng Zhanfeng
It is fascinating to explore the distribution of CO 2 hydrogenation products regulated by heterogeneous catalysts, as both the chemical state of surface metals and structure of the support itself of the supported catalysts may affect the performance of CO 2 hydrogenation. Herein, the complete switching of CO 2 hydrogenation products from CH 4 to CO can be realized by induction of Cl into Ru/TiO 2 catalyst. Density functional theory (DFT) calculations indicated that Cl ions were mainly located on the Ru metal sites of Ru/TiO 2 catalysts. Bader charge analysis and Ru 3p X-ray photoelectron spectra (XPS) results suggested that electrons transferred from Ru to Cl, resulting in the decrease of electron density of Ru. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of CO 2 hydrogenation and CO adsorption proved that with the increase of the Cl ion content, the adsorption of CO on the catalyst surface was significantly weakened, and resulted in the high CO selectivity. Our work demonstrates the role of Cl ions in regulating the distribution of CO 2 hydrogenation products, and provides new ideas for regulating other catalytic processes.
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ACS Catalysis
·
2022
·
IF 13.7
Xiwen Song,Chengsheng Yang,Xianghong Li,Zhongyan Wang,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong
Understanding the nature of adsorbates and intermediates on catalytic surfaces is critical for the development of highly efficient systems for CO2 conversion. However, the role of structural hydroxyl groups in CO2 hydrogenation is still under debate. This paper describes an experimental study on the nature of surface-bound hydroxyl groups over Al2O3-supported Cu catalysts for CO2 reduction. A model 5 wt % Cu/Al2O3 catalyst with stable hydroxyl groups was prepared. The structural hydroxyl groups were modulated by the hydration of unsaturated Al3+ sites, which were introduced by the evaporation-induced self-assembly method. Terminal hydroxyl groups (T-OH*) were found to significantly facilitate the conversion of CO2, while the AlVI-T-OH and AlIV-T-OH species promoted the formation of Al-b-HCOO and Al-m-HCOO species, respectively, accompanied with the increase in methanol and dimethyl ether yields. The reaction behavior of hydroxyl species was further investigated by in situ IR experiments with HD isotope exchange on Cu/Al2O3. T-OH* were identified as active sites participating in the formation of key intermediates, while more hydroxyl sites were occupied by formate species with the H coadsorbed on the Cu surfaces.
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Membranes
·
2023
·Vol. 13
·期 2
·166
·
IF 4.2
Jingfeng Li,Zeyu Cao,Bo Zhang,Xinai Zhang,Jinchao Li,Yaping Zhang,Hao Duan
CO is a significant product of electrochemical CO2reduction (ECR) which can be mixed with H2to synthesize numerous hydrocarbons. Membranes, as separators, can significantly influence the performance of ECR. Herein, a series of quaternized polybenzimidazole (QAPBI) anion exchange membranes with different quaternization degrees are prepared for application in ECR. Among all QAPBI membranes, the QAPBI-2 membrane exhibits optimized physico-chemical properties. In addition, the QAPBI-2 membrane shows higher a Faraday efficiency and CO partial current density compared with commercial Nafion 117 and FAA-3-PK-130 membranes, at −1.5 V (vs. RHE) in an H-type cell. Additionally, the QAPBI-2 membrane also has a higher Faraday efficiency and CO partial current density compared with Nafion 117 and FAA-3-PK-130 membranes, at −3.0 V in a membrane electrode assembly reactor. It is worth noting that the QAPBI-2 membrane also has excellent ECR stability, over 320 h in an H-type cell. This work illustrates a promising pathway to obtaining cost-effective membranes through a molecular structure regulation strategy for ECR application.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Huanni Xia,Hua Jin,Yating Zhang,Hao Song,Jianqiao Hu,Yun Huang,Yanshuo Li
Membrane technology with environmentally friendly and cost-efficient features has been well acknowledged as a promising solution for effective CO 2 separation. Metal organic framework (MOF) glasses are one of the most attractive membrane materials currently, because of their easy processability, absence of grain-boundary defects, and permanent porosity. In this study, a mixed linker tetrahedral imidazolate framework-4 (TIF-4) MOF with ultrahigh glass forming ability was selected for fabricating highly CO 2 selective membranes. Through adjusting the molar ratio of the imidazole (Im) and 5-methylbenzimidazolate (5-mbIm) linkers in the TIF-4 framework, the melting temperatures as well as the CO 2 adsorption property could be controlled systematically. After vitrification, TIF-4 glasses (a g TIF-4) with varying 5-mbIm content were prepared, and all of them exhibit higher isosteric heat of CO 2 adsorption than the corresponding TIF-4 crystals. Both CO 2 /CH 4 and CO 2 /N 2 uptake ratio (298 K, 1 bar) of a g TIF-4 samples are more than twice as that of TIF-4 crystals, suggesting the great potential of a g TIF-4 for CO 2 separation. Further, a g TIF-4 membranes were successfully prepared by the melt-quenching process from the polycrystalline membranes. a g TIF-4 membranes are highly CO 2 selective with CO 2 /N 2 and CO 2 /CH 4 separation factors of 27 and 30. More importantly, a g TIF-4 membrane displays long-term stability up to 10 months, which is highly conductive to its industrial application for CO 2 separation.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1287-1291
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IF 2.726
Gong Yu,Pan Jing,Zhang Lingling,Wang Xiao,Song Shuyan,Zhang Hongjie
Electrochemical reduction of carbon dioxide into value-added products is a promising way to recycle the greenhouse gas, thus solving the crisis of global warming. Pressing challenges remain in regulating the catalytic selectivity. In this work, we demonstrated a metal-organic frameworks-assisted approach to synthesizing In species loaded on the surface of N doped carbon matrix. By controlling the particle sizes, the catalytic selectivity can be easily altered. The obtained In c /NC possesses the outstanding capability for converting CO 2 into CO. And 80.09% Faraday efficiency (FE) of CO can be achieved at 0.8 V vs. RHE. While the In 2 O 3 /C exhibits different catalytic behaviors, the main product is formic acid and the FE is more than 50% at 0.8 V vs. RHE. The selectivity reversal can be attributed to the strong interactions between In clusters and N atoms of carbon supports, which efficiently inhibits the formation of the by-product, formic acid. Our research has paved a new way to modulate catalytic selectivity by manipulating the fine structures of the catalysts.
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ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200188
·
IF 9.14
Chengjin Li,Xiaoxia Zhou,Qingming Zhang,Yi Xue,Zhaoyu Kuang,Han Zhao,Chung-Yuan Mou,Hangrong Chen
Graphical CO 2 to formic acid : A novel kind of Sn/TiO 2 /Si photocathode is developed for CO 2 reduction reaction (CO 2 RR), which shows excellent selectivity to HCOOH under applied potential. The improved light performance and heterojunction composite structure, together with the modulated electronic configuration, co-contribute to the high CO 2 RR performance. Using renewable energy to convert CO 2 into liquid products, as a sustainable way to produce fuels and chemicals, has attracted intense attention. Herein, a novel heterostructured photocathode composed of Si wafer, TiO 2 layer, and Sn metal particles has been successfully fabricated by combining of a facile hydrothermal and electrodeposition method. The obtained Sn/TiO 2 /Si photocathode shows enhanced light absorption performance by the surface plasmon resonance effect of Sn metal. Especially, the Sn/TiO 2 /Si photocathode together with rich oxygen vacancy defects jointly promote photoelectrochemical CO 2 reduction, harvesting a high faradaic efficiency of HCOOH and a desirable average current density (−4.72 mA cm −2 ) at −1.0 V vs. reversible hydrogen electrode. Significantly, the photocathode Sn/TiO 2 /Si also shows good stability due to the design of protecting layer TiO 2 . This study provides a facile strategy of constructing an efficient photocathode to improve the light absorption performance and the electron transfer efficiency, exhibiting great potential in the CO 2 reduction.
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Journal of Energy Chemistry
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2022
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IF 13.599
Zhiyan Si,Cederick Cyril Amoo,Yu Han,Jian Wei,Jiafeng Yu,Qingjie Ge,Jian Sun
Catalytic conversion of CO 2 to high-value products is a crucial method to achieve targets of carbon dioxide emissions peak and carbon neutralization. However, realizing a controllable product distribution in a single CO 2 hydrogenation process is of great challenge. Herein, we prepared the CuFe nanoalloy catalyst that directly transforms CO 2 to alkanes using physical sputtering method in mild condition. The characteristic results show that the proximity between Cu and Fe is the crucial factor to tunable products among the different catalysts. The formation of unique coordination of FeCu 4 nanoalloys from high-energy sputtering process provides close interaction between Cu and Fe, which is favorable to formation of low carbon paraffin, however, a distant proximity and weak interaction will increase the selectivity of olefins and alcohols. This work provides a general strategy for tuning target chemicals and enriches the viewpoints in CO 2 hydrogenation.
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BRAZILIAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 39
·期 3
·661-669
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IF 1.772
Jin Zhengwei,Yu Changjun,Wang Ruyang,Wei Wei,Jing Yunhuan,Wang Qi
The production of precipitated calcium carbonate (PCC) from carbonate-free minerals and CO 2 from industrial exhaust gas could lower energy consumption and promote CO 2 sequestration. The present study proposes a chemical looping process for the production of PCC from wollastonite (calcium silicate) and CO 2 from industrial exhaust using ammonium chloride as the looping medium; this study also included a pilot setup with a capacity of 3 kg of carbonate per hour to demonstrate the process. The process consisted of three phases: extraction of calcium from the wollastonite with hydrochloric acid; carbonation of the CO 2 in the extract solution in the presence of ammonia to produce calcium carbonate while generating ammonium chloride; and regeneration of hydrochloric acid and ammonia by the decomposition of ammonium chloride. A special air-lift reactor with an integrated settling vessel was designed for the carbonation reaction. The extraction and carbonation conditions were optimized, and fine calcium carbonate with a purity greater than 98% and a particle size of 2 μm was produced. The overall utilization of the calcium from wollastonite and the CO 2 reached 99 and 90%, respectively. This process avoids the high-temperature pyrolysis of limestone and thus consumes less energy. It also sequesters CO 2 from industrial exhaust and is a green and high-performing process for the production of PCC.
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高影响因子
FUEL
·
2022
·
IF 8.035
Huangyu Yan,Guojie Zhang,Ying Xu,Qiqi Zhang,Jun Liu,Guoqiang Li,Yuqiong Zhao,Ying Wang,Yongfa Zhang
In recent years, amine functionalized materials have attracted great interest as prospective solid adsorbents for CO 2 capture. However, the amine functionalization of traditional supports (such as SBA-15, etc.) can lead to a decrease in the pore volume and specific surface area of the adsorbent, which significantly affects the CO 2 adsorption–desorption kinetics. To overcome this problem, the macro-/mesoporous multimodal pore silica was quickly synthesized using a ternary nonionic surfactant as a template through a partitioned collaborative self-assembly method, and impregnated with TEPA. The prepared support HMS-4 h has bimodal pores (pore size of 9.41 nm and 90 nm), which can not only improve the dispersibility of the loaded TEPA, but also effectively reduce the diffusion resistance of CO 2 . At the same time, the high surface area (838 m 2 /g) and large pore volume (2.34 cm 3 /g) of HMS-4 h can further improve the adhesion and quantity of amine-based active sites. The highest adsorption capacity reaches 6.04 mmol/g for HMS-4 h-75%TEPA at 90 ℃ and 1 bar. The adsorption capacity for HMS-4 h-75%TEPA was steady after 10 adsorption–desorption cycles. BET, XRD, FT-IR, SEM, TG-DTG were used to characterize the performance of the adsorbent. The CO 2 adsorption mechanism and the effects of organic amine loading, adsorption temperature and CO 2 concentration on CO 2 adsorption performance were systematically studied. The research shows that HMS-4 h-75%TEPA is an excellent adsorbent with high adsorption capacity in a wide temperature range, and low energy. This provides a reference for the design of high-performance solid amine CO 2 adsorbents in the future.
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GREEN CHEMISTRY
·
2022
·Vol. 24
·期 4
·1561-1569
·
IF 11.034
Peixuan Wu,Xinchao Wang,Ruhui Shi,Haiyang Cheng,Fengyu Zhao
The synthesis of self-healing and recyclable polymeric materials from renewable CO2 is of great importance in the fields of functional materials and sustainable chemistry. In this work, mechanically robust poly(urea-imine) (PUI) thermosets were prepared from CO2-sourced oligourea (OUa), terephthalaldehyde (TA) and tri(2-aminoethyl)amine (TAEA) through condensation between equimolar amino and aldehyde groups. The synthesized PUIs have satisfactory mechanical performance, seal-healing and recyclable properties as they contain cross-linked dynamic imine bonds and reversible hydrogen bonds. These properties can be adjusted by changing the ratio of TAEA to OUa, thus varying the chemical bonds and chain structure. The highest values for the mechanical properties tensile stress (10.2 MPa) and Young's modulus (79 MPa) were obtained in a PUI thermoset synthesized from a molar ratio of TAEA to OUa of 3 : 2 (OUa2-T3). In addition, this thermoset can be healed at 80 °C with a healing efficiency over 92% owing to the high reversibility of imine and hydrogen bonds and the flexibility of CO2-sourced OUa chains. Moreover, it can also be reprocessed and recycled by physical and/or chemical means without change in its chemical structure, glass transition temperature and original mechanical properties. Additionally, this PUI thermoset can be easily degraded into its original reagents OUa, TA and TAEA under acid conditions. Therefore, as novel sustainable materials, the PUI thermosets reported in this article have great potential to replace conventional non-degradable thermosets over a wide field.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yafei Sang,Zhe Shu,You Wang,Lizhi Wang,Du Zhang,Qin Xiao,Fa Zhou,Jianhan Huang
A series of bifunctional ionic hyper-cross-linked polymers were synthesized by the Friedel-Crafts reaction and ionic post-functionalization. The as-prepared polymers had high Brunauer-Emmett-Teller surface areas ( S BET , 623–1345 m 2 /g), considerable bifunctional ionic groups, namely bromide anions, and carboxyl groups. The polymer namely DHI-CSU-3-Br had a good CO 2 capture capacity (134 mg/g, 273 K, and 1.0 bar), moderate isotopic adsorption heat (28–38 kJ/mol), and excellent CO 2 cycloaddition ability. The catalytic experiments showed that 99% of propylene oxide was successfully converted to cyclic carbonate (70 °C, 0.1 MPa CO 2 , and 4 h). The catalytic activity of the polymer was easy to be recovered and it was repeatedly reused 5 times without significant reduction. This synthetic strategy for the preparation of the bifunctional ionic hyper-cross-linked polymers provided an alternative approach for CO 2 capture and catalytic conversion.
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