APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Tengfei Zhang,Peng Zheng,Fangna Gu,Wenqing Xu,Wenxing Chen,Tingyu Zhu,Yi-Fan Han,Guangwen Xu,Ziyi Zhong,Fabing Su
Hydrogenation of CO 2 into CH 4 is an effective strategy for dealing with CO 2 -relevant environmental problems. Since the CO 2 methanation reaction involves multiple electron transfers and various C1 intermediates, improving the reaction rate at each step is critical to accelerating the entire reaction. Here, we report a dual-active-site tandem catalyst (Ru 1 Ni/CeO 2 ) composed of Ru single atoms (Ru 1 ) and Ni nanoparticles , which can effectively convert CO 2 to CH 4 , showing ∼90% CO 2 conversion and ∼99% CH 4 selectivity at 325 °C, much higher than those of the Ru 1 /CeO 2 and Ni/CeO 2 catalysts. Experimental and theoretical calculation results reveal that Ru 1 is extremely active for converting CO 2 to CO, while the Ni site is highly efficient for the subsequent sequential CO to CH 4 reaction step. The coexistence of the Ru 1 and Ni sites significantly boosts the overall reaction. This work offers a promising strategy for the rational design of efficient multisite tandem catalysts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Pengxin Zeng,Chuanwen Zhao,Chenxi Liang,Peiyu Li,Haoxuan Zhang,Ruilin Wang,Yafei Guo,Hongqiang Xia,Jian Sun
K 2 CO 3 -based adsorbent pellets produced by graphite-casting method are promising alkali metal-based solid CO 2 adsorbents. The incorporation of porous metal oxide supports is an effective to enhance CO 2 adsorption capacity of K 2 CO 3 -based adsorbent pellets. In this work, graphite-casted K 2 CO 3 -based adsorbent pellets incorporated with different porous supports (i.e., TiO 2 , ZrO 2 , and SiO 2 ) were prepared for CO 2 capture. Comparatively, the ZrO 2 -supported, K 2 CO 3 pellets loaded with 30 wt% of K 2 CO 3 exhibit the highest CO 2 adsorption capacity, approximately 0.93 mmol/g. For the SiO 2 -supported K 2 CO 3 adsorbent pellets, the high calcination temperature (>700 °C) required to remove the graphite layer covering the pellet surface will cause the formation of new eutectics (i.e., K 2 Si 2 O 5 and K 2 Si 4 O 9 ), which leads to the collapse of the adsorbent pellets. Low calcination temperature of 500 °C can avoid the collapse of the SiO 2 -supported K 2 CO 3 adsorbent pellets and remove most of the graphite on the surface. Moreover, the CO 2 adsorption capacity can be further increased to 1.30 mmol/g by adding 20 wt% of microcrystalline cellulose to the SiO 2 -supported K 2 CO 3 adsorbent pellet. Although the adsorption capacity of structurally improved, SiO 2 -supported K 2 CO 3 pellets is still inferior to that of structurally improved, ZrO 2 -supported K 2 CO 3 pellets, they exhibit great cost advantage. Therefore, SiO 2 -supported K 2 CO 3 pellets with 20 wt% of microcrystalline cellulose have industrial application prospects.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Wen-Feng Zhou,Yi-Min Wei,Zhi-Wei Xiao,Yan Jiang,Yan-Kai Zhang,Zhen-Wei Zhang,Hui Hu,Longlong Geng,Da-Shuai Zhang,Yong-Zheng Zhang,Xiuling Zhang,Shujuan Zhuang
A new dual-cage-based porous metal-organic framework (MOF, termed DZU-113) assembly from the triazole-carboxylate linker and the Cu(II) paddle-wheel unit was solvothermally constructed. The structure of DZU-113 was determined by single-crystal X-ray diffraction, being consisted of the octahedral cage with an internal diameter of approximately 0.4 nm, and the spindle nano-cage with internal pores of about 0.8 nm × 2.2 nm, respectively. Specially, the uncoordinated N atoms of triazole groups are distributed in the bottleneck windows of the spindle nano-cage, serving as open functional sites. DZU-113 has permanent porosity with the Brunauer−Emmett−Teller surface area of 1207 m 2 g −1 . The CO 2 adsorption test demonstrated that the total uptake of DZU-113 can reach 66.7 cm 3 g −1 at 298 K, and 112.0 cm 3 g −1 at 273 K, 1 bar. Moreover, it achieves robust catalytic performance for the cycloaddition of CO 2 and epoxides under mild conditions.
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高影响因子
FUEL
·
2022
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IF 8.035
Leilei Xu,Chunying Xu,Bin Chen,Yufang Bian,Xueying Wen,Ge Cheng,Cai-e Wu,Jian Qiu,Mindong Chen
In this work, a series of hexagonal mesoporous silica (HMS) confined Ni-based CO 2 methanation catalysts were successfully synthesized by the facile one-pot strategy. In the Ni-HMS system, the metallic Ni active sites were embedded in the framework of HMS support. Hence, the metallic Ni active sites were highly dispersed and stably confined by the HMS framework. The kinetic study demonstrated that the Ni-HMS catalysts behaved much lower apparent activation energy than the 15Ni/HMS and 15Ni/SiO 2 catalysts, accounting for their enhanced low-temperature activities. Meanwhile, the online TPSR and in-situ DRIFTS of the CO 2 methanation were employed to study the reaction intermediates over these catalysts. The CHOO–, CH x O-, and CO x were considered as the reaction intermediates over the Ni-HMS catalysts and the possible reaction pathways were also proposed. In conclusion, the Ni-HMS catalysts were considered as a series of efficient and stable catalyst candidates for CO 2 methanation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yun Long,Jian Sun,Changnian Mo,Xiangyao She,Pengxin Zeng,Hongqiang Xia,Jubing Zhang,Zijian Zhou,Xinming Nie,Chuanwen Zhao
Calcium looping (CaL) belongs to a promising high-temperature CO 2 capture technology because of adopting cheap and extensive source CaO-based sorbents . However, CaO-based sorbents are prone to occur the issues of sintering and elutriation in the fluidized-bed reactors. To further enhance the practicability, the Zr-supported, CaO-based sorbent pellets were produced using the graphite-moulding method. Different synthesis modes (i.e., sol-gel, hydration-mixing, and wet-mixing) were compared for preparing CaO-based composite slurry before pelletization. Sol-gel is the promising synthesis mode to prepare Zr-supported, CaO-based pellets with outstanding CO 2 capture performance due to achieving a more uniform distribution of inert CaZrO 3 spacer. Moreover, the Zr-based stabilizer content within sorbent pellets produced by the combined method of sol-gel and graphite-moulding was further studied. The higher content of Zr-based stabilizer promotes the enhancement of cyclic stability and mechanical strength of Zr-supported, CaO-based pellets. After 17 cycles, the sorbent pellets containing 20 wt% of Zr-based stabilizer display a high CaO carbonation conversion of 74.1 %. Moreover, CaO-based pellets with 20 wt% of Zr-based stabilizer possess a higher compression strength of 4.84 ± 1.08 MPa, which is as high as 1.8 times that of the pellets with 5 wt% of Zr-based stabilizer.
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PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 5
·2565-2578
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IF 1.843
Cai Zhaotian,Guo Xiaoxuan,Zhang Lixiang,Xiao Guomin
This work reports the synthesis of Zinc porphyrin-based porous (POP-ZnTPP) by a typical Yamamoto-Ullmann coupling reaction, which exhibited abundant tiny nanopores, excellent CO 2 adsorption capacity, and CO 2 /N 2 selectivity. The open pore environment of POP-ZnTPP facilitated the exposure of active sites, which intensified the catalytic activity in the cycloaddition reaction of epoxides (PO) with CO 2 under mild conditions. As expected, POP-ZnTPP catalyst completely converted PO to cyclic carbonates (COCs) at ambient temperature (25 °C, 1.5 MPa). It is also worth noting that POP-ZnTPP could convert PO into COCs under the simulated flue gas (15% CO 2 and 85% N 2 , v/v) atmosphere, which is very favorable for industrial applications of CO 2 . In addition, POP-ZnTPP catalyst as one of the most outstanding catalysts exhibited excellent broad substrate scope and remarkable reusability. This work has a certain guiding significance for developing an environmentally friendly COC production process.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Su Liu,Mingqiang Tang,Jun Pang,Jintao Hu,Weijie Chen,Jie Cheng,Zewei Liu,Haihong Zhao,Rong Tan
Water-soluble single-chain polymeric nanoparticles (SCPNs), which isolated catalytic sites within a hydrophobic interior, made water-incompatible organometallic catalysis highly efficient in water. However, it is still a great challenge to conveniently control their hydrophilicity, so as to combine reactivity and recovery of the catalytic SCPNs in aqueous systems. Herein, we have developed a series of catalytic SCPNs, which possessed CO2-switchable hydrophilic/hydrophobic behavior, to realize the gas-controlled reaction and separation for asymmetric sulfa-Michael addition (SMA) in water. A novel series of CO2-switchable random copolymers were thus synthesized by copolymerization of CO2-responsive amidine derivatives with hydrophobic chiral salen FeIII monomers via reversible addition-fragmentation chain transfer polymerization. Characterization suggested their CO2-controlled self-collapse behavior in water due to CO2-switched change in hydrophilicity/hydrophobicity of the amidine moiety. The resultant CO2-switchable SCPNs provided hydrophobic, catalytic compartments for asymmetric SMA in water upon CO2 addition, giving various chiral β-keto sulfides with almost quantitative yields (90–98%) and high enantioselectivities (93–99%). When CO2 is removed by N2 bubbling, they were collapsed and spontaneously precipitated from the aqueous system for steady reuse. The gas-controlled reaction-separation approach provides an energy-efficient way to combine reactivity and recovery of catalytic SCPNs in aqueous systems, which should be quite practical in large-scale industrial applications.
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Asian Journal of Organic Chemistry
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2022
·Vol. 11
·期 8
·e202200234
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IF 3.116
Yifei Ye,Yanglin Chen,Junzhe Huang,Jianmin Sun
Graphical A series of functionalized ionic liquids (ILs) immobilized on B-doped mesoporous SiO 2 catalysts were fabricated for effectively converting CO 2 into cyclic carbonates under metal-absent and cocatalyst-free conditions A series of functionalized ionic liquids (ILs) immobilized on B-doped mesoporous SiO 2 catalysts were fabricated for effectively converting CO 2 into cyclic carbonates under metal-absent and cocatalyst-free conditions. Functionalized imidazolium ILs were in-situ synthesized by Debus-Rdziszewski imidazole reaction. Among the prepared catalysts, 5B−SiO 2 −NH 2 −3−I catalyst owing to the synergistic effects of nucleophile, Lewis acid-base and hydroxyl hydrogen bond donors in the catalyst, presented the better catalytic activity for propylene epoxide to the product of propylene carbonate with 99% yield and selectivity at 110 °C and 2 MPa CO 2 . The catalyst also displayed moderate yield for various mono-substituent epoxides. Besides, the gradual decline in the product yield during consecutive runs could be easily refreshed by aqueous acidic solution washing.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Daoyun Zhu,Haiou Liu,Yangqiang Huang,Xiao Luo,Yu Mao,Zhiwu Liang
Rare earth metal oxides are known to have good catalytic effectiveness in the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol. In this work, we screened ceria (CeO2) catalysts by analyzing their capacity for CO2 adsorption. The effects of the crystal surface morphology and oxygen vacancy on the catalytic performance of the ceria catalyst were studied by using density functional theory (DFT). The results show that the (110) surface and higher oxygen vacancy content can better promote the synthesis of DMC and that the rod-shaped CeO2 catalyst has a better catalytic effect. The oxygen vacancy content on the catalyst was improved by freeze-drying and confirmed by thermogravimetric analysis, Raman spectroscopy, and electron paramagnetic resonance. The freeze-dried CeO2 (CeO2-FD) then showed a higher catalytic performance. The conversion rate of methanol and the yield of DMC were 33.95% and 584 mmol g–1cat, respectively, under mild conditions (140 °C and 1 MPa).
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高影响因子
APPLIED CLAY SCIENCE
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2022
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IF 5.907
Jiangtao Peng,Ruifeng Guo,Xiongxi Shi,Peiping Zhang,Fagui Qiu,Wenqing Li,Cundi Wei,Shiding Miao
A type of clay-supported catalysts was developed for cycloaddition of CO 2 by immobilizing metal-free ionic liquids (IL) on ball clay (BC) via a one-step strategy. The metal-free IL was loaded on the surface of BC via thermal and acid treatment. The synthesized materials (IL@P-BC) were characterized by Fourier transform infrared spectroscopy (FTIR), N 2 adsorption-desorption, and transmission electron microscopy (TEM). The composite IL@P-BC demonstrated excellent catalytic performance (yield 94.0%, selectively >99%) for coupling of CO 2 with epoxides to produce cyclic carbonates under the lack of any co-catalyst. The good recyclability and excellent suitability were obtained for the composite IL@P-BC. These experimental analyses deepen comprehension of the rational design of clay-based catalysts for CO 2 cycloaddition, further confirmed ball clay was a promising support.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Anbang He,Yong Yang,Qiang Zhang,Ming Yang,Qian Zou,Jun Du,Changyuan Tao,Zuohua Liu
Electrochemical reduction of CO 2 to C2 products on Cu-based catalysts provides a promising approach for controlling the global carbon balance and restoring renewable surplus electricity. The enhanced CO 2 adsorption and CO local concentration are beneficial for CO 2 conversion and C2 intermediates formation, promoting the progress of CO 2 utilization. Here, we report a bimetallic MOF-derived Co 3 O 4 -CuO x /C (M-CuCo/C) catalyst constructed with Co 3 O 4 and CuO x sites wrapped in the carbon skeleton, achieving efficient CO 2 activation and C2 generation under low overpotential. The optimized M-CuCo/C catalyst (Cu/Co ratio of 1:2) exhibits a total current density of 19.28 mA/cm 2 at −1.05 (V vs. RHE), which is 8.60 times than that on MOF-derived CuO x /C (M-Cu/C). The highest C2 faradic efficiency (FE) reaches 79.2% (-0.75 V vs. RHE), accompany with a C2 production rate of 275.6 μmol/(g·h). The special nanorods-like morphology assembled by dual sites significantly increases electrochemical surface area and electron transmission rate during eCO 2 RR. The local CO intermediates under real-time electrochemical environment are monitored via rotation ring disk electrode (RRDE) techniques. Combined with in situ infrared measurements and DFT studies, it’s demonstrated that CO 2 could be efficiently converted to CO under low overpotential on Co 3 O 4 sites, forming local CO-enriched environment around neighboring CuO x sites and further accelerating the process of C2 formation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Yunxia Bai,Mei Li,Xuemei Liu,Jinyu Han,Xinli Zhu,Qingfeng Ge,Hua Wang
Photocatalytic CO2 reduction is a promising route to simultaneously address two critical issues related to the energy and environment. Herein, a direct Z-scheme photocatalytic system, Ti3+ defective TiO2/CdS nanoflowers, was fabricated to enhance the production of C1–C3 products from CO2 reduction. First, nanoflower-like TiO2 (NF-TiO2) is prepared using a TiB2 precursor to build in Ti3+ defects. Then, the NF-TiO2/CdS heterojunctions are constructed via the sulfurization of TiO2/Cd-MOF. Importantly, the optimal heterojunction photocatalyst NF-TiO2/CdS0.6 exhibits a highly promoted CO2 reduction activity not only for CO and CH4 but also for C2–C3 hydrocarbons. The cumulative yields of CO and CH4 are 1007.0 μmol/g and 83.5 μmol/g (2.5 h), respectively, and a yield of 55.3 μmol/g (2.5 h) of C2–C3 hydrocarbons is obtained. This enhanced yield of C1–C3 products is attributed to the synergistic effects of abundant Ti3+ defects that increase adsorption and activation of CO2, the large surface area that provides sufficient active sites, and a direct Z-scheme heterojunction with a good intimate contact interface that effectively separates charge carriers and accumulates electrons with strong reducibility. Moreover, the photoluminescence analysis of hydroxyl radicals was conducted to provide evidence for the direct Z-scheme mechanism. This work provides a facile method for the construction of a TiO2-based direct Z-scheme photocatalytic system for improving photocatalytic performance toward CO2 reduction.
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