Nature Communications
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2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Zhou Jun,Gao Zhe,Xiang Guolei,Zhai Tianyu,Liu Zikai,Zhao Weixin,Liang Xin,Wang Leyu
Supports can widely affect or even dominate the catalytic activity, selectivity, and stability of metal nanoparticles through various metal-support interactions (MSIs). However, underlying principles have not been fully understood yet, because MSIs are influenced by the composition, size, and facet of both metals and supports. Using Ru/TiO 2 supported on rutile and anatase as model catalysts, we demonstrate that metal-support interfacial compatibility can critically control MSI modes and catalytic performances in CO 2 hydrogenation. Annealing Ru/rutile-TiO 2 in air can enhance CO 2 conversion to methane resulting from enhanced interfacial coupling driven by matched lattices of RuO x with rutile-TiO 2 ; annealing Ru/anatase-TiO 2 in air decreases CO 2 conversion and converts the product into CO owing to strong metal-support interaction (SMSI). Although rutile and anatase share the same chemical composition, we show that interfacial compatibility can basically modify metal-support coupling strength, catalyst morphology, surface atomic configuration, MSI mode, and catalytic performances of Ru/TiO 2 in heterogeneous catalysis.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Yi Liu,Ying Chen,Yunli Liu,Zewen Chen,Huan Yang,Zhongxiao Yue,Qing Fang,Yunfei Zhi,Shaoyun Shan
Solar energy is considered as the cleanest, cheapest, and most sustainable energy source, and CO 2 cycloaddition that is drove by solar energy has unique advantages in the aspect of energy and environmental. Therefore, Zn and N co-doped porous carbon nanosheets (ZNCs), which were synthesized by a simple one-step pyrolysis method, as catalysts and photothermal material to photothermally drive cycloaddition of CO 2 . The prepared ZNCs show graphene-like layered structure, uniformly distributed Lewis acid (Zn atoms) sites and Lewis base (N atoms) sites, full spectrum absorption and high photothermal conversion efficiency. More importantly, ZNCs have a higher catalytic efficiency than traditional heating methods because it can be quickly in-situ heated by light, hence the yield of cyclic carbonate reached 91.1% (0.1 MPa CO 2 , 1000 mW·cm −2 full-spectrum irradiation, 12 h). ZNCs were recycled five times without significant reduction in catalytic efficiency, and have high activity to other series of epoxides. A possible CO 2 cycloaddition mechanism which is catalyzed by ZNCs is proposed, including the step of adsorption, ring opening, insertion and cyclic carbonates formation.
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Sustainable Materials and Technologies
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2022
·
IF 10.681
Boshu Jiang,Qiming Sun,Bachirou Guene Lougou,Hao Zhang,Xian Li,Zhibin Qu,Yong Shuai,Chi-Hwa Wang
The solar-driven thermochemical CO 2 conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality . However, finding a material with excellent thermal stability, oxygen exchange capacity, and CO selectivity is one of the most important challenges in the thermochemical CO 2 conversion approach. This study investigated the solar thermochemical CO 2 -splitting characteristics through the synergistic thermal catalytic activity of CuO and NiFe 2 O 4 and the effect of SiC photothermal properties. The thermochemical redox cycling performance of CO 2 conversion through thermally activated catalysts was experimentally investigated via thermogravimetric combined quantum chemical calculations to provide comprehensive insights into the physicochemical principles underlying the thermochemical catalytic CO 2 -splitting. The X-ray diffraction, scanning electron microscopy, and energy spectrum detector technics were developed to gain detail on the crystal structure, surface morphology , and chemical composition changes in the reacting media. The newly synthesized composite material consisting of 25%CuO and 75%NiFe 2 O 4 (CNF-13) coated SiC porous skeleton resulted in higher CO 2 -splitting catalytic activity with an instantaneous CO production of 10.98mL ⋅ min ‐1 g CNF‐13 −1 and direct CO 2 -to-CO conversion rate of 33.9% at 1000–1200 K reaction temperature. The thermochemical CO 2 -splitting activity and redox stability of CNF-13@SiC was promoted by the photothermal properties of SiC support and the formation of Cu 2 O and Fe 3 O 4 new active material phases easing CO 2 reduction at low energy. This study provided experimental and theoretical findings that can be used as guidance for the fundamental research and application of CO 2 catalytic conversion into fuels through a solar thermochemical driven strategy.
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DALTON TRANSACTIONS
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2022
·Vol. 51
·期 20
·7950-7956
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IF 4.569
Liuyong Chen,Jun Yang,Wenqian Yang,Jiahui Xian,Guangqin Li
Photochemical CO2 conversion into carbon fuel is a promising route to explore renewable energy and relieve climate change. However, it is still a key challenge to achieve high selectivity to CO and simultaneously achieve high conversion efficiency in photochemical CO2 reduction. Herein, we demonstrate the effect of Ni metal centers as catalytic active sites for the photocatalytic conversion of CO2 to CO by designing and constructing Ni metal–organic framework (Ni-MOF) materials. In pure CO2, Ni-MOF catalyst exhibits outstanding performance for visible-light-driven reductive CO2 deoxygenation with a high CO evolution rate of 19.13 μmol h−1 (per 1 mg of catalyst) and CO selectivity of 91.4%, which exceeds those of most reported systems. Upon using isostructural Co-MOF as the catalyst to replace Ni-MOF, a moderate performance towards CO2 photoreduction and low CO selectivity (40.1%) were observed, implying that the performance of CO2 photoreduction and CO selectivity are dependent on unsaturated metal centers.
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ChemSusChem
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2022
·Vol. 15
·期 7
·e202200184
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IF 9.14
Siyong Ou,Min Zhou,Wen Chen,Yuyao Zhang,Yueli Liu
Graphical Photocatalytic CO 2 reduction : A COF-5/CoAl-layered double hydroxide (LDH) heterojunction photocatalyst is developed for the CO 2 reduction reaction. CoAl-LDH incorporation enhances the visible-light response-ability of the photocatalyst and improves the separation efficiency of photogenerated electron–hole pairs through the role of a type-II heterojunction. Photocatalytic conversion of CO 2 into value-added chemical fuels is an attractive route to mitigate global warming and the energy crisis. Reasonable design of optical properties and electronic behavior of the photocatalyst are essential to improve their catalytic activity. Herein, the 1D/2D heterojunction by direct in-situ synthesis of the covalent organic framework (COF)-5 colloid on the surface of CoAl layered double hydroxide (LDH) was used as the prospective photocatalyst for CO 2 reduction. COF-5/CoAl-LDH nanocomposite achieved 265.4 μmol g −1 of CO with 94.6 % selectivity over CH 4 evolution in 5 h under visible light irradiation, which was 4.8 and 2.3 times higher than those of COF-5 colloid and CoAl-LDH, respectively. The enhanced catalytic activity was derived from the increased visible-light activity and the construction of type II-2 heterojunction, which greatly optimized visible light harvesting and accelerated the efficient separation of the photoinduced holes and electrons. This work paves the way for rational design of heterojunction catalysts in photocatalytic CO 2 reduction.
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CHEMICAL ENGINEERING SCIENCE
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2022
·
IF 4.889
Pan Ma,Meili Ding,Xi Liu,Wei Rong,Jianfeng Yao
Metal-organic framework (MOF) derived porous carbons are known as desirable catalysts for carbon dioxide (CO 2 ) catalytic conversion. However, practical CO 2 utilization processes are severely hampered by their powder form and relatively poor activities. Herein, we demonstrate the rational synthesis of ZnO and/or metallic Co embedded in N-doped porous carbon by one-step pyrolysis of bimetallic MOF, Co/Zn-ZIF. The optimized catalyst exhibits remarkable activity and recyclability towards the coupling reaction of CO 2 and epoxides owing to hierarchical pore, good CO 2 uptake and sufficient active sites. More importantly, its catalytic performance can be well maintained even under dilute CO 2 (15%), humid environment or light irradiation instead of heating. These results pave a way to develop highly efficient materials for practical CO 2 catalytic conversion.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Xinyi Wan,Kuiyuan Zhang,Ting Wan,Youguo Yan,Zhizhen Ye,Xinsheng Peng
The emergence of Newton's cradle is promising for fast substance transport, which attracts tremendous attentions for industrial applications. Herein, an ultrafast and highly selective nano Newton's cradle for CO 2 transport is constructed through the assembly of negatively charged graphene oxide (GO) nanosheets and positively charged zinc hydroxide nanostrands (ZHNs), followed with impregnation of ionic liquid (IL) within the nanochannels. The GO laminates provide robust structure for whole system. The incorporation of IL endows the membrane with sieving ability to different gases while ZHNs play a key role to accelerate selective CO 2 adsorption, thus achieving exceptional CO 2 separation performance. The resulted nano Newton's cradle demonstrates that a huge CO 2 permeance enhancement of more than 53 times as that of the GO/IL membrane without ZHNs, superhigh CO 2 /light gases selectivities (35 for CO 2 /H 2 , 194 for CO 2 /CH 4 and 331 for CO 2 /N 2 ), out-stripping the Robeson upper bound of traditional polymeric membranes , as well as long-term operation stability. This innovative strategy not only provides an outstanding candidate for carbon capture, but also opens a new avenue to design separation membranes with high performance for various applications.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
·
IF 3.656
Cong Liu,Qibin Zhu,Zhonghui Zhu,Chen Sun,Yimin Xuan,Kai Zhang
Foreigner element doping is one of effective strategies to promote photocatalytic reaction. Herein, a convenient one-step solvothermal method is applied to enable the isomorphic substitution of In 3+ in In(OH) 3 by Bi 3+ . The composition and microstructure of the photocatalysts were mainly obtained by X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM). UV–Vis diffuse reflectance and photoluminescence (PL) spectroscopy revealed the optical properties of photocatalysts. The surface properties of photocatalysts were mainly characterized by X-ray photoelectron spectroscopy (XPS). Theoretical calculations were used to reveal the reaction mechanism. The results indicated that CO production rate and selectivity of Bi 3+ doped In(OH) 3 are much higher than that of the pure In(OH) 3 , which could be attributed to the extended solar spectral response, the enhanced CO 2 adsorption capacity and the accelerated photogenerated carriers separation. The current work verifies the potential application of isomorphic substitution as an efficient route for solar fuel production.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Menglei Mao,Tingting Zhai,Lingding Meng,Zihui Meng,Wenfang Liu
Enzymatic conversion of CO 2 to high-value chemicals is a significant route for the utilization of greenhouse gases in mild, high-selectivity and environment-friendly way, however, conversion efficiency is not yet satisfying. Here, mesoporous silica (mSiO 2 ) nanoparticles with controllable structure were prepared and modified by polydopamine (PDA) and polyethyleneimine (PEI), which were then used in an integrated process for CO 2 capture and conversion to formate for the first time. The effects of structure parameters of mSiO 2 and modification conditions on its application properties were investigated. The results show that in a range of 230 ∼ 500 nm, SiO 2 particles with smaller size exhibited better intensifying effect, while the optimal size was 410 nm for mSiO 2 with the same etching extent, attributed to a higher specific surface area. mSiO 2 itself was a robust CO 2 adsorbent and the addition of 0.01 g mSiO 2 (410) enabled CO 2 conversion to be accelerated 11.94 times compared to free enzyme. After modification, with 0.05 g PDA/PEI-mSiO 2(340) and PDA/PEI-mSiO 2(410) , the enzyme reaction was expedited up to 24 and 30.8 times of the system without particles due to an enhanced CO 2 uptake, as a collaborative result of mesoporous structure and amino-functionalization. Following that, PDA/PEI-mSiO 2(410) was used as the carrier for the co-immobilization of formate dehydrogenase and carbonic anhydrase, which could retain 86.7% activity after use for 10 times and 55.2% activity after 21 days at 4 °C, while 29.6% for free enzymes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Luming Qi,Wanyong Yang,Linlin Zhang,Qing Liu,Zhaoyang Fei,Xian Chen,Zhuxiu Zhang,Jihai Tang,Mifen Cui,Xu Qiao
Additive introduction based on porous amine-silica hybrid materials is one of the key technologies to enhance the ability of CO2 capture. Hence, we first developed a one-step strategy of directly introducing brush-like cetyltrimethylammonium chloride (CTAC) and bis-(γ-triethoxysilylpropyl)-tetrasulfide (BTES) additives into the silica support to prepare micro-mesoporous organosilica nanoparticles with double brush-like additives modified (MMON-D). Then, the amine-functionalized CO2 adsorbent (MMON-D-50) was obtained via tetraethylenepentamine impregnation. The adsorbent with double additives exhibited a higher CO2 adsorption performance (4.04 mmol/gadsorbent and 0.33 mmol CO2/mmol N under pure CO2 and 25 °C conditions) than that of the adsorbents with none or a single additive. Furthermore, spectra analysis, kinetics, and adsorption heats were performed to clarify the adsorption mechanism of the synergistic action of CTAC and BTES. The results revealed that CTAC as a quaternary ammonium formed on the adsorbent surface can facilitate the formation of carbamic acid. Meanwhile, BTES as a swelling agent endows silica support with a large pore size and inhibits the formation of silylpropyl carbamate to enhance CO2 adsorption performance. This work supplies a novel surface-modified strategy for developing adsorbents with excellent CO2 capture performance, which is of prime importance for both academic interests and practical applications.
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Journal of CO2 Utilization
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2022
·
IF 8.321
Junhui Liu,Bing Li,Junying Cao,Chunshan Song,Xinwen Guo
Conversion of CO 2 to value-added chemicals by hydrogenation is considered as a promising way for CO 2 utilization. Addition of promoters into iron-based catalysts is a crucial strategy to enhance the catalytic performance in CO 2 hydrogenation. In this work, indium (In) was introduced into iron-based catalyst as a promoter to improve the conversion efficiency of CO 2 . The promotional effects of In on CO 2 hydrogenation were also studied by varying In loading. In promoter can accelerate the reduction of ferric oxide in iron-based catalysts. The evolution of In species had a significant influence on iron species during reaction, leading to the obvious induction period for the In-promoted catalysts with more than 3 wt% In loadings. Addition of In enhanced the adsorption of CO 2 , and obviously improved the CO 2 conversion. The CO selectivity over In-promoted catalysts slightly decreased, while the distribution of hydrocarbons changed a little. The CO 2 conversion over 10Fe2In1K/Al 2 O 3 increased 17% compared with that over the benchmark 10Fe1K/Al 2 O 3 catalyst. The insights into the promotional effects of In provides a value choice to design iron-based catalysts for CO 2 hydrogenation.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 101
·期 2
·657-670
·
IF 2.5
Yu Zhang,Jing Cai,Xiao-Sen Li,Zhao-Yang Chen,Gang Li
To investigate the effect of the particle size of porous media on CO 2 hydrate formation, the formation experiments of CO 2 hydrate in porous media with three particle sizes were performed. Three kinds of porous media with mean particle diameters of 2.30 μm (clay level), 5.54 μm (silty sand level), and 229.90 μm (fine sand level) were used in the experiments. In the experiments, the formation temperature range was 277.15–281.15 K and the initial formation pressure range was 3.4–4.8 MPa. The final gas consumption increases with the increase in the initial pressure and the decrease in the formation temperature. The hydrate formation at the initial formation pressure of 4.8 MPa in 229.90 μm porous media is much slower than that at the lower formation pressure and displays multistage. In the experiments with different formation temperatures, the gas consumption rate at the temperature of 279.15 K is the lowest. In 2.30 and 5.54 μm porous media, the hydrate formation rates are similar and faster than those in 229.90 μm porous media. The particle size of the porous media does not affect the final gas consumption. The gas consumption rate per mol of water and the final water conversion increase with the decrease in the water content. The induction time in 5.54 μm porous media is longer than that in 2.30 and 229.90 μm porous media, and the presence of NaCl significantly increases the induction time and decreases the final conversion of water to hydrate.
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