ACS Applied Energy Materials
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2021
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IF 6.024
Yuyao Zhang,Wen Chen,Min Zhou,Guobin Miao,Yueli Liu
Photoreduction of CO2 into useable hydrocarbon fuels has been widely used in the energy conversion field. However, the high carrier recombination rate and the low conversion efficiency of as-prepared catalysts greatly restrict their photocatalytic application. Herein, we synthesize Ti3C2/CsPbBr3 quantum dot (Ti3C2/CsPbBr3 QD) composites by the method of self-assembly, which are used in the photoreduction of CO2. As a result, Ti3C2/CsPbBr3 QD composites exhibit excellent photocatalytic activity and stability for the photocatalytic CO2 reduction. Especially, the generation rate of CO (17.98 μmol h–1 g–1) for Ti3C2/CsPbBr3 QD composites is 9.37 times higher than that of CsPbBr3 QDs (1.92 μmol h–1 g–1), and 97.35% of the activity is still retained after three consecutive cycles. The improved photocatalytic performance is mainly attributed to the construction of the type II-2 heterojunction as the built internal electric field (IEF) in the p–n junction could accelerate the separation for both photoinduced holes and electrons. Therefore, this work provides an insight into the construction of heterojunction photocatalysts with halide perovskite QD materials for photocatalytic applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yan Zhang,Haryo Wibowo,Li Zhong,Mika Horttanainen,Zunbo Wang,Caimeng Yu,Mi Yan
High CO 2 content exists in the raw syngas produced from supercritical water gasification of food waste, CO 2 removal to improve quality of the syngas is necessary before further utilization. In this study, Cu-BTC, Mg/Cu-BTC, Cu-BTC@MWCNT, and Mg/Cu-BTC@MWCNT were synthesized and characterized as CO 2 adsorbents. The adsorption experiments were conducted to investigate the optimal adsorbent and adsorption conditions. The results indicated that Mg 2+ and multi-walled carbon nanotubes (MWCNT) doped into Cu-BTC influenced the physical properties of adsorbents. Among of all studied adsorbents, Mg/Cu-BTC@MWCNT had the maximum CO 2 adsorption capacity (3.63 mmol/g) and selectivity (14.28) at 25 °C and 100 kPa. Analysis of variance (ANOVA) exhibited that adsorption pressure had significant effects on CO 2 adsorption capacity of Mg/Cu-BTC@MWCNT. The influences of different operating parameters on CO 2 adsorption capacity and selectivity were discussed in Mg/Cu-BTC@MWCNT. The adsorption isotherms of gas components on Mg/Cu-BTC@MWCNT can be sorted as follows: CO 2 > CO > CH 4 > H 2 . In additional, the regeneration experiment with 5 times was conducted and the result showed that Mg/Cu-BTC@MWCNT has high stability.
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Journal of CO2 Utilization
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2021
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IF 7.132
Ziyi Zhao,Xiaotong Li,Jianghao Wang,Xiangzhou Lv,Hao Bin Wu
Electrochemical reduction of carbon dioxide to value-added fuels offers a promising method to solve increasingly serious environmental problems and alleviate energy crisis. Herein, we report a facile method by coating Cu electrode with CeO 2 nanoparticles to largely enhance the C 2+ products selectivity during CO 2 electroreduction. The Faradaic efficiency of C 2+ products for optimal CeO 2 -coated Cu electrode reached a high value of 61 % at -1.05 V vs RHE, and exhibited good stability for over 9 h of CO 2 electrolysis. The CeO 2 nanoparticles were found to induce oxidative corrosion of the Cu foil, leading to a CuO x layer in contact with the CeO 2 nanoparticles. The interface between CeO 2 nanoparticles and oxide-derived Cu might be attributed to the enhanced catalytic activity for C 2+ products by promoting the C C coupling process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xinyue Ma,Jianjun Du,Hao Sun,Fenghui Ye,Xin Wang,Pengfei Xu,Chuangang Hu,Lipeng Zhang,Dong Liu
Efficient and cost-effective electrocatalysts for CO 2 reduction with high selectivity are desirable but remain challenging. Herein, a low-cost and efficient electrocatalyst composed of boron, nitrogen co-doped mesoporous carbon (BNMC) for CO 2 reduction reaction (CO 2 RR) along with the catalytic mechanism are reported. The resultant BNMC (i.e., BNMC-1000) exhibits good CO 2 RR activity with high Faradaic efficiency (FE, 95%) towards CO at low overpotential (423 mV). It is demonstrated that the codoping of nitrogen and boron atom, and the mesopore structure are favorable to the excellent catalytic activity of CO 2 RR. The doped boron atom cooperate with nitrogen atom could adjust the projected density of states of the carbon active site generating a proper adsorbed energy of *COOH and *CO on the carbon surface. This work offers a basic guide for developing metal-free carbon-based CO 2 RR electrocatalysts with high-performance.
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JOURNAL OF MATERIALS SCIENCE
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2021
·Vol. 56
·期 28
·15653-15666
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IF 4.22
Zhang Nan,Zhang Yaoming,Duan Chunjian,Li Song,Yang Zenghui,Zhang Xinrui,Wang Tingmei,Wang Qihua
Traditional “top-down” methods for graphene preparation, like micromechanical cleavage and ultrasound methods, usually cannot preserve both efficiency and quality simultaneously. Herein, we provide an environmental-friendly graphene exfoliating method with high efficiency and high quality that combines the microfluidization process (liquid phase) and supercritical carbon dioxide process (gas phase), namely the dual-phase exfoliating (DPE) method. The combination of effective tangential force (shearing force) and normal force (push and pull), which are originally from microfluidization and supercritical carbon dioxide process, respectively, maximizes the exfoliating efficiency. The DPE method offers a high yield of up to 70.25% for graphene preparation (941.04 g per day theoretically), while the graphene sheets could remain single or a few layers (> 80%) and around micron size. By molecular dynamic simulations, it is theoretically proved that carbon dioxide can intercalate between graphite layers and expand the interlayer spacing under supercritical conditions. This DPE method, by combining the advantages of different phase processes, provides an ideal process design perspective for large-scale preparation of other 2D materials.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2021
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IF 6.064
Ying Yang,Kai Chen,Liang Huang,Min Li,Taiping Zhang,Mi Zhong,Ping Ning,Junya Wang,Shikun Wen
It has been reported that the addition of graphene oxide (GO) can increase the dispersion and heterogeneous nucleation of layered double hydroxide (LDH), thus providing more active sites, which is more conducive to CO 2 adsorption. Herein, we reported alkali metal nitrates ((Li 0.3 Na 0.18 K 0.52 )NO 3 ) promoted LDH and GO composites (LDH/GO) as adsorbents for CO 2 capture. The influence of mass ratio of LDH to GO, the impregnation ratio of alkali metal nitrates, the calcination and adsorption temperature, as well as the cycling stability were investigated systematically. The results indicated that the CO 2 capture capacity of LDH/GO composite with 30 mol% (Li 0.3 Na 0.18 K 0.52 )NO 3 could reach 4.51 mmol·g −1 , which was 5.86 times higher than LDH/GO1 without loading alkali metal nitrates. Moreover, it had outstanding CO 2 adsorption capacity in the range from 200 °C to 320 °C. In addition, the cyclic adsorption and desorption test manifested that the CO 2 uptake of the material can reach 3.07 mmol·g −1 after 22 cycles. We believe that this study will give a significant contribution to fabrication of LDH based composites as CO 2 adsorbents in future study.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xiangdong Kong,Jingwen Ke,Zhiqiang Wang,Yan Liu,Yibo Wang,Weiran Zhou,Zhengwu Yang,Wensheng Yan,Zhigang Geng,Jie Zeng
A typical mode of CO 2 activation is that d electrons at the d orbital of transition metals transfer to the unoccupied π * orbital of CO 2 . Thus the exploration of the relationship between d -electron behaviors and CO 2 activation is of great importance. Herein, we demonstrate that high-spin state of 3 d electrons in Co 2+ facilitated the activation of CO 2 over Co-salophen-X (X represents to Cl, Br, or I). Among these catalysts, Co-salophen-Br exhibited the highest Faradaic efficiency for CO. Notably, the Faradaic efficiency for CO over Co-salophen-Br reached 98.5 % at −0.70 V versus reversible hydrogen electrode, which was 1.5 and 1.2 times as high as those over Co-salophen-Cl (64.8 %) and Co-salophen-I (81.8 %), respectively. Density functional theory calculations revealed that high-spin state of Co sites decreased the reaction energy barrier for the formation of CO. Based on the analysis of electronic state, the ratio of high-spin state was 65.6 % for Co-salophen-Br, which was the highest among the three Co-based molecules. The Co sites with high-spin state promoted the electron transfer from high-energy 3 d orbital (3 d z2 and 3 d x2-y2 ) of Co to the unoccupied π * orbital of CO 2 , improving catalytic performance.
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Catalysis Science & Technology
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2021
·Vol. 11
·期 10
·3422-3427
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IF 6.119
Yuqing Shao,Xinkui Wang,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Pang,Qiang Xu,Min Ji,Min Wang
Solar-driven CO2 conversion into fuels and sustainable energy has attracted increasing attention around the world. However, the efficiency of the transformation remains relatively low due to the rapid recombination of photogenerated charge carriers. In this work, we prepared a ZnIn2S4–ZnAlOx nanocomposite for visible light driven CO2 reduction. The thin layered structure facilitated the photoinduced charge carrier separation and transfer, and also gave excellent adsorption ability towards CO2 molecules. Such a nanocatalyst exhibited excellent activity in visible-light driven CO2 reduction with a CO optimal formation rate of 1100 μmol g−1 h−1, which is 5 times that over bulk ZnIn2S4, and the CO/H2 ratio was increased from 0.2 over bulk ZnIn2S4 to 1.5 over the ZnIn2S4–ZnAlOx composite. In situ FT-IR experiments indicated that CO2 was reduced on ZnIn2S4–ZnAlOx following a COOH* pathway. This work gives insights into the mechanism of the photocatalytic CO2 reduction reaction and inspiration to construct novel heterostructure materials for application in energy and environmental catalysis.
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ACS Applied Nano Materials
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2021
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IF 5.097
Zhi Liu,Jia Zheng,Lianfeng Duan,Zhi Zhu
CO2 photoreduction into high-valued fuels is considered as a promising route to alleviate the clash between the environment and energy. Morphology-dependent CeO2 nanocrystallines with special crystal planes and increased amounts of specific surface areas, structural defects, and active sites have recently demonstrated excellent performance in catalysis. In this article, a biomass-assisted synthesis of CeO2 (BC) photocatalyst is successfully synthesized via a simple yet effective hydrothermal-calcining method by using commercial Ce(NO3)3 as a precursor and leaves of Alternanthera philoxeroides (LAP) as a crystal growth modifier. The amount of LAP introduced into the precursor has a significant effect on regulating the growth of the formed CeO2 from nanocubes to nanorods for the resulting BCs. Owing to the emergence of the just right microenvironment for regulating the growth of the CeO2 nanocrystalline, the optimal sample of BC-15 with a morphology of nanorods is found to be the most efficient one as a photocatalyst for CO2 reduction under visible light. As the major product, the CO yield (126.8 μmol g–1 at a reaction time of 6 h) of BC-15 is ∼7.4-fold of the reference CeO2 nanocubes synthesized without LAP in the precursor. In addition, the underlying evolution process of the nanorods and detailed mechanism insight into the boosted CO2 photoreduction performance are investigated by means of a series of experimental characterizations and results. The present work provides a meaningful protocol to utilize the crystal phase engineering strategy to design morphology dependence of photocatalysts and assisted synthesis with renewable biomass materials for solar-to-fuel conversion.
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REACTIVE & FUNCTIONAL POLYMERS
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2021
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IF 3.975
Yunfan Zhang,Jialin Liu,Jingbo Zhao,Zhiyuan Zhang
A new and simple method was established to prepare polyamides with a chelating feature through Michael addition and polycondensation . A piperazine-diester monomer , that is, N,N´-bis(methyl propanoate) piperazine (BMPZ), was synthesized through a Michael addition of piperazine and methyl acrylate . Three polyamides containing piperazine rings (PIP-PAs) were synthesized via melt polycondensation from BMPZ and different diamines. PIP-PAs were modified by chelating Co 2+ , and several PIP-PA-Co 2+ complexes were obtained. The structure of BMPZ and PIP-PAs was characterized by FT-IR and 1 H NMR spectra. DSC and wide angle X-ray diffraction verified the crystallizable feature of PIP-PAs. They possessed T m from 81 °C to 171 °C, tensile strength up to 31 MPa, and good toughness. Chelating PIP-PAs with Co 2+ was accompanied by color change and the loss of crystallization. The effect of chelation on T g , tensile strength, and Young's modulus was investigated. Polyamide complexes with good mechanical property and solvatochromic feature were synthesized successfully.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Mingpu Kou,Wei Liu,Yongye Wang,Jindi Huang,Yanli Chen,Ying Zhou,Yi Chen,Minzhi Ma,Kai Lei,Haiquan Xie,Po Keung Wong,Liqun Ye
The application of covalent organic framework (COF) for photocatalytic CO 2 conversion has received more and more attention. However, it is still a challenge for photocatalytic conversion of CO 2 with atmosphere concentration to high added value hydrocarbons products (C x H y ) such as CH 4 and C 2 H 4 . Here, integrating the advantages of micropore structure and single atom catalysis, we introduced single- atom MoN 2 sites into COF to construct Mo-COF materials. The aberration-COrrected high-angle annular dark-field scanning transmission electron microscopy (HAADF- STEM) confirms that Mo single atom on COF. Mo-COF can reduce CO 2 to C x H y under visible light with a selectivity of 42.92 % and C 2 H 4 product was found for the the first time. In-situ fourier transform infrared spectrometer (In situ FT-IR) and theoretical calculation showed that the introduction of single-atom MoN 2 sites is the key to improving the catalysis performance. It also provides a new idea for converting CO 2 into high added value C x H y products.
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Molecular Catalysis
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2021
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IF 5.062
Rui Tang,Niamat Ullah,Yajun Hui,Xin Li,Zhenhua Li
Carbon dioxide hydrogenation for value-added chemicals has been regarded as a promising way for CO 2 utilization. This paper describes the preparation of Ni/CeO 2 catalysts derived from Ce-MOF precursor by impregnation or one-pot method and their application in carbon dioxide methanation. Various techniques were employed to characterize the prepared catalysts, including N 2 adsorption–desorption, X-ray diffraction (XRD), Raman spectroscopy, field emission scanning electron microscopy (SEM), H 2 -temperature programmed reduction (H 2 -TPR), H 2 -temperature programmed desorption (H 2 -TPD) and CO 2 -temperature programmed desorption (CO 2 -TPD). The results showed that compared with commercial CeO 2 and CeO 2 prepared by precipitation, CeO 2 derived from Ce-MOF exhibited more oxygen vacancies and lower temperature reducibility, making it more beneficial for the adsorption and activation of CO 2 . Consequently, nickel supported on rod-shaped CeO 2 derived from Ce-MOF exhibited higher CO 2 conversion and methane selectivity at low temperatures. Furthermore, the Ni/CeO 2 −M-1 catalysts prepared by one-pot method showed superior activity since nickel could be partially incorporated into ceria lattice, leading to the formation of Ce 1-x Ni x O 2-y solid solutions and oxygen vacancies. The effect of nickel loading on the properties of the catalysts by one-pot method was also investigated, and the optimum Ni loading was 15 wt.% owing to the maximum number of oxygen vacancies being reached.
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