CATALYSIS COMMUNICATIONS
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2022
·
IF 3.51
Bin Chen,Jian Qiu,Liang Xu,Yan Cui
The Ni/Ce 0.8 Zr 0.2 O 2 catalysts with different Ni doping amounts (5 wt%, 10 wt%, 15 wt%, 20 wt%, and 25 wt%) are prepared by the impregnation technique and used as CO 2 methanation catalysts in this work. The effects of various Ni doping loading on CO 2 methanation catalytic performance at low temperatures were investigated in this catalytic system. The results show that the catalyst with 15 wt% Ni doping shows the best catalytic performance. Since the heated sintering of Ni nanoparticles was prevented efficiently by CO 2 methanation, these mesoporous catalysts exhibit excellent stability. Therefore, the catalyst is expected to be an efficient CO 2 methanation catalyst at low temperatures.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Feifei You,Yunan Zhou,Danyang Li,Hao Zhang,Dawei Gao,Xiaohong Ma,Rui Hao,Juzhe Liu
Photoreduction of CO 2 to value-added chemicals and fuels is an attractive solution to alleviate environmental problems and energy crisis at the same time. However, engineering efficient photocatalysts with high activity and product selectivity is still challenging. Herein, we achieved three-dimensional (3D) spatial configuration design at micro-scale and heterogeneous interface construction at nano-scale on a SnS 2 /SnO 2 composite, which featured hierarchical flower-like morphology consisted of nanosheets and type-II semiconductor structure . It behaved excellent selectivity and impressive photocatalytic CO 2 -to-CO performance with a yielding rate of 60.85 μmol g -1 h −1 , roughly 3 times higher than that of SnS 2 and was in the front rank of this kind catalysts under 300 W Xe lamp illumination without using any sensitizers or noble metals . The enhanced catalytic capability could be attributed to the elaborately built structure with suitable energetic position that afforded effective separation and migration of photo-generated electron/hole pairs as well as enhanced light caption and absorption. Meanwhile, main reactive intermediates (e.g., CO 2 – and *COOH) were captured by in-situ Fourier transform infrared spectroscopy (FTIR), suggesting a fluent catalytic pathway on the SnS 2 /SnO 2 platform. This work provides a new scheme to build advanced catalysts based on multiscale design and rational phase assembling.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xinru Zhang,Xiaofeng Ren,Yonghong Wang,Jinping Li
Mixed matrix composite membranes (MMCMs) for CO 2 capture have great potential in carbon neutral goal. However, simultaneous enhancement in permeance and selectivity is very difficult, since mismatching pore and chemical structures of filler with polymer matrix are the stumbling block. Herein, novel core–shell MOFs@COFs hybrids were prepared by growing hierarchical pore covalent organic frameworks (COFs, nitrogen-enriched nanoporous polytriazine (NENP)) on the surface of metal organic framework (MOFs, zeolite imidazolate framework-8 (ZIF-8)), where ethylenediamine were impregnated into NENP pore to adjust the chemistry environment of the shell. Subsequently, a porous polysulfone (PSf) membrane-supported MMCMs were developed by a coating method using a mixed dispersion of ZIF-8@NENP-NH 2 and polyvinylamine (PVAm), which was used to efficiently separate CO 2 from N 2 . The rough COFs layer (NENP-NH 2 ) was closely wrapped on the smooth surface of ZIF-8 as identified by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and N 2 adsorption. Even-distributed ZIF-8@NENP-NH 2 had well miscibility with the PVAm matrix from hydrogen bonding as evidenced by SEM, attenuated total reflectance-FTIR and differential scanning calorimetry. The CO 2 permeance as high as 301 GPU accompanied with a selectivity of 91 was obtained for MMCMs loaded with 7 wt% ZIF-8@NENP-NH 2 , which were enhanced by 296.1% and 89.6%, respectively, when compared with the pristine PVAm membrane, transcending 2019 upper bound. We assume that the surface chemistry environment in hierarchical pore of the shell and molecular sieving pore in the core in the short-range order facilitate CO 2 permeation. Furthermore, this membrane maintained an average CO 2 permeance of 369 GPU and a CO 2 /N 2 selectivity of 97.3 for over 360 h using CO 2 /N 2 mixed gas as feed gas.
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Nano-Micro Letters
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2022
·Vol. 14
·期 1
·1-16
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IF 23.655
Qiu Chen,Qian Kun,Yu Jun,Sun Mingzi,Cao Shoufu,Gao Jinqiang,Yu Rongxing,Fang Lingzhe,Yao Youwei,Lu Xiaoqing,Li Tao,Huang Bolong,Yang Shihe
For electrochemical CO 2 reduction to HCOOH, an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density ( J HCOOH ) at a low overpotential. Indium oxide is good HCOOH production catalyst but with low conductivity. In this work, we report a unique corn design of In 2 O 3- x @C nanocatalyst, wherein In 2 O 3- x nanocube as the fine grains dispersed uniformly on the carbon nanorod cob, resulting in the enhanced conductivity. Excellent performance is achieved with 84% Faradaic efficiency (FE) and 11 mA cm −2 J HCOOH at a low potential of − 0.4 V versus RHE. At the current density of 100 mA cm −2 , the applied potential remained stable for more than 120 h with the FE above 90%. Density functional theory calculations reveal that the abundant oxygen vacancy in In 2 O 3- x has exposed more In 3+ sites with activated electroactivity, which facilitates the formation of HCOO* intermediate. Operando X-ray absorption spectroscopy also confirms In 3+ as the active site and the key intermediate of HCOO* during the process of CO 2 reduction to HCOOH.
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PubMed
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Journal of CO2 Utilization
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2021
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IF 7.132
Bowen Lu,Yongqing Xu,Zewu Zhang,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang
Cu-based catalysts had been widely used in CO 2 hydrogenation process for their excellent performance and high selectivity. Micron-sized Cu powder obtained by ball milling exhibited poor CO 2 activity for its large particle size and small specific surface area, limited its catalytic application. In this work, micron Cu powder was modified with CeO 2 species synthesized from different cerium precursor salts via a solution auto-combustion method to investigate CO 2 hydrogenation activity. This work revealed that CeO 2 species formed from cerium acetate precursor salt achieved excellent CO 2 performance (1.64 mol/g cat .h at 400 °C), which was 3.8 times and 6000 times higher than that from cerium nitrate salt or cerium chloride salt, respectively. Interestingly, a thick dense CeO 2 shell would be formed on micron Cu generated from cerium(III) chloride precursor salt, which inhibited CuO x reduction and had the opposite effect for RWGS reaction. In addition, the CuO x species in CeO 2 @Cu synthesized from cerium chloride salt resulted in the CH 4 selectivity. The enhancement performance of the CeO 2 @Cu prepared from cerium acetate salt and cerium nitrate salt could be attributed to the oxygen defects formed around the Cu-Ox-Ce interface area and metallic Cu in the RWGS reaction. Cerium precursor salts enhanced the structural integrity of CeO 2 @Cu and played a vital role in RWGS reaction. These results will support a new direction for exploring micron Cu powder in Cu-based catalysts for CO 2 utilization.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Tingyan Lu,Qian Li,Jiawei Shao,Linlin Wang,Ruixue Pang,Xiaying Wu,Xin Hu
Backgrounds Adsorption by adsorbents is accepted as a promising technology that can efficiently separate CO 2 from flue gas. Optimal adsorption performance can be obtained by specific solid adsorbents with excellent CO 2 adsorption capacity. Methods In this work, N, S co-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile synthesis process i.e. hydrothermal treatment followed by KOH activation. N, S enriched hydrochar was obtained after hydrothermal treatment of polyacrylonitrile fiber and ammonium sulfide. Further KOH activation of hydrochar obtained N, S co-doped carbons with advanced porous structure. Significant findings This series of sorbents has the highest CO 2 uptake of 3.37 and 5.23 mmol g −1 at 1 bar, 25 °C and 0 °C, respectively. Detailed investigation revealed that the mutual effects of narrow microporostiy, N and S content are responsible for the CO 2 uptake of these adsorbents. Additionally, these adsorbents also show various good CO 2 capture properties such as excellent recyclability, reasonable CO 2 /N 2 selectivity, moderate heat of adsorption, fast adsorption kinetics, and good dynamic adsorption capacity. These findings suggest that N, S co-doped porous carbons derived from polyacrylonitrile fiber are potential promising sorbents for CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Biao Zhu,Qianxin Xu,Xiaoyan Bao,Hao Yin,Yumei Qin,Xing-Can Shen
Sunlight-driven photocatalytic CO 2 into useful carbon compounds is an ideal way to mitigate the greenhouse effect. However, this strategy is limited by poor light absorption and rapid photoexcited electron-hole recombination of traditional photocatalysts. Here, a g-C 3 N 4 (CN) foam/LDH heterojunction monolith (NCF) was fabricated by growing NiFe-LDH in situ on the porous CN foam substrate. The composite had good air permeability and light transmittance, which improves light-harvesting, CO 2 capture, and interfaces charge transfer of the NCF. The results show that the NCF catalyst has good CO 2 adsorption performance (1.52 mmol g −1 ) and enhanced CO 2 photoreduction activity (55.1 μmol g -1 h −1 ), which is ∼ 10 times higher than that of pure LDHs powder. Furthermore, the practical applicability of the NCF monolith with different thicknesses is illustrated via the CO 2 photoreduction test for the first time. This work could shed light on the development of dual-functional materials for efficient capture and photoreduction of CO 2 .
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EUROPEAN POLYMER JOURNAL
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2021
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IF 4.598
Sun-Chang Xi,Hao-Nan Guo,Chang-Yuan Yang,Ren Wang,Dong-Yue Wang,Bin Dong
In this work, an aromatic nitrile containing the pyrimidine moiety and bisimidazolium cations (PyImCl) was synthesized and subsequently employed to prepare a bisimidazolium-based cationic covalent triazine framework (PyImCl-cCTF) through the ionothermal trimerization reaction. The chemical composition and structure of PyImCl-cCTF were carefully revealed by a series of techniques. As examined by N 2 sorption isotherms at 77 K, PyImCl-cCTF exhibited large surface area and abundant microporous structures. Together with the high content of imidazolium cations derived from the bisimidazolium-based monomer, PyImCl-cCTF showed high CO 2 uptake capacity of 235 and 133 mg/g at 1 bar under 273 and 298 K, respectively, superior to the previously reported cCTFs. The dye adsorption performance of PyImCl-cCTF was performed for commonly used dyes. Surprisingly, PyImCl-cCTF exhibited a certain removal effect on both anionic and cationic dyes. Moreover, PyImCl-cCTF with the positively charged skeleton can quickly remove anionic dyes through electrostatic interactions, showing almost 100% removal efficiency within 20 min. These results demonstrate that PyImCl-cCTF can behave as an efficient adsorbent for both CO 2 capture and dye removal to solve environmental problems.
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ChemCatChem
·
2021
·Vol. 13
·期 23
·4931-4936
·
IF 5.686
Cuizhu Huo,Xinxing Cao,Zixian Ye,Yu Li,Tongbu Lu
Graphical Foam supported : The hierarchical bimetallic electrocatalyst comprising Cu foam-supported bundle-like structure with thin amorphous SnO shell (Sn-24 h@CB) was successfully synthesized for highly efficient electrocatalytic reduction of carbon dioxide. An unprecedented partial current density of C1 products (CO and HCOOH) up to 128.6 mA cm −2 was achieved with a Faradaic efficiency of ∼80 % in H-type cell. Renewable electricity-driven reduction of CO 2 into value-added chemicals has been recognized as a promising sustainable energy conversion method to achieve carbon-neutrality. Although Sn-based catalysts show excellent selectivity towards CO and HCOOH in CO 2 reduction, the reaction activity, i. e. current density, remains quite low (<100 mA cm −2 ). Herein, a hierarchical bimetallic electrocatalyst consisting of Cu foam-supported bundle-like structure and thin amorphous SnO layer was fabricated for efficient electroreduction of CO 2 to C1 products (CO and HCOOH). The hierarchical structure ensured higher large electrochemically active surface area, while the thin amorphous SnO layer could efficiently adsorb CO 2 , and stabilize the *CO 2 − intermediate formed in the rate-determining step, thereby boosting the reaction activity of CO 2 reduction. As a result, an unprecedented partial current density of 128.6 mA cm −2 was achieved for C1 products at −1.4 V vs. RHE with a Faradaic efficiency of 79.2 % in an H-type cell. The strategy of integrating optimized structure with active site here may be beneficial to other related energy conversion systems.
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Catalysis Science & Technology
·
2021
·Vol. 12
·期 2
·606-612
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IF 6.119
Yuqing Shao,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Ji,Min Pang,Min Wang,Xinkui Wang
The photocatalytic reduction of CO2 into valuable fuels and sustainable energy has a promising future, yet remains a challenge due to low charge separation efficiency and inadequate active sites. We find that ZnIn2S4-loaded secondary amine-functionalized organic silica (ZnIn2S4/NH–SiO2) was effective for visible-light driven CO2 photocatalytic reduction. The ZnIn2S4/NH–SiO2 with 40% ZnIn2S4 content achieves a CO production rate of 1304.8 μmol g−1 h−1 at room temperature, which is about 3 times higher than that of pristine ZnIn2S4. The thin ZnIn2S4 nanosheet accelerates the separation of photogenerated electron pairs, and the amine groups on ZnIn2S4/NH–SiO2 act as active sites for adsorption and activation of CO2, hence facilitating the photoreduction of CO2.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shi-Qing Wang,Xu Gu,Xinzhu Wang,Xiao-Yu Zhang,Xiao-Yao Dao,Xiao-Mei Cheng,Jing Ma,Wei-Yin Sun
Defects in MOFs can benefit light absorption and charge transfer for photocatalytic application, nevertheless, studies on interplay between structural defects and photocatalytic properties of MOFs are in infancy. Herein, a series of UiO-66-NH 2 with different kinds of defects were created for regulating CO 2 photocatalytic reduction. Theoretical calculations in combination with experimental data verified that the sample with ligand-vacant (UiO-66-NH 2 -LV) defect performed better than non-defect, missing-cluster and monocarboxylate compensated ones in the photocatalytic CO 2 reduction reactions. UiO-66-NH 2 -LV shows superior photocatalytic activity with the highest CO yield of 30.5 μmol g −1 h −1 , which is 9.2 times higher than that of the sample with missing-cluster (UiO-66-NH 2 -MC), as well as the highest quantum yield (QY) of 0.90%. DFT calculations further demonstrate the correlation between discriminative photocatalytic activities in defect structures and tunable electronic properties characterized by absorption energy, E abs , and charge transfer energy, E LMCT , in the photocatalytic process. The ligand-vacant defect with the lowest sum of E abs and E LMCT will lower photocatalytic reaction energy barrier in the rate-limiting step among the elementary reaction step during CO 2 photoreduction. The insights gained from this study will guide the MOFs defect-engineering for enhancing CO 2 photocatalytic capacity.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Xiaodong Zhang,Yajiao Zhou,Hang Zhang,HuangJingWei Li,Kang Liu,Hongmei Li,Hao Pan,Junhua Hu,Junwei Fu,Shanyong Chen,Min Liu
Formate is an important liquid chemical, which can be produced by electrocatalytic carbon dioxide reduction reaction (CO 2 RR). Most of the metal catalysts for CO 2 RR to formate are toxic or noble metals, such as Cd, Hg, Pb and Pd, leading to the environmental pollution or increased production costs. Herein, we develop an environmentally friendly and low-cost NiZn alloy catalyst for CO 2 RR to formate. The X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) confirm the alloy structure of the prepared NiZn catalyst. As for a catalyst for CO 2 RR, the NiZn alloy exhibits the FE HCOO - (Faraday efficiency of HCOO – ) of 36 ± 0.7% at − 0.9 V vs. RHE in 0.1 M KHCO 3 , and remarkable stability for 40,000 s at − 0.8, −0.9, −1.0 and − 1.1 V vs. RHE, respectively. Theoretical calculation results indicate that the NiZn alloy exhibits the middle valence electron structure between the Zn and Ni metal, resulting in the favorable pathway for HCOOH formation but unfavorable for the hydrogen evolution reaction and CO production. The Ultraviolet Photoelectron Spectroscopy results verify the modulated valence electron structure for NiZn alloy as compared to Ni and Zn, consistent with the theoretical calculation results. This work provides new insights into design of alloy catalysts for CO 2 RR to formate.
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