APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Honglin Li,Shoufu Cao,Hongman Sun,Yonglian Lu,Ying Zhang,Xiaoqing Lu,Jingbin Zeng,Zifeng Yan
Copper (Cu) has been proved as an efficient catalyst in carbon dioxide electrochemical reduction reaction (CO 2 RR) towards hydrocarbons, but still suffers from low selectivity and poor stability. Herein, Cu-based/CxNy catalysts were fabricated by facile pyrolysis of CuNCN in sealed quartz tubes. It is found that CuNCN pyrolyzed at 300 °C (CuNCN-300) exhibits a high C 2 H 4 Faradaic efficiency of 48.5% at 500 mA cm - 2 . However, increasing the pyrolysis temperature above 400 °C gives rise to CH 4 being the predominant product and CuNCN-500 achieves CH 4 Faradaic efficiencies of 66.3% at 300 mA cm - 2 . Combining experimental and DFT calculation results, Cu 3 N plays a crucial role in the formation of C 2 H 4 , while tri-s-triazine units in CuNCN-500 reduce the barrier of *CO hydrogenation to *CHO and retard C-C coupling on Cu surface. These findings mark the significance of precise tailoring of the synergistic effect between g-C 3 N 4 and different Cu species for achieving the desired selectivity during CO 2 RR.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2022
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IF 6.437
Zijun Yi,Chao Li,Lijun Zhang,Shu Zhang,Wenran Gao,Shuang Wang,Bin Li,Xun Hu
CO 2 can be used to activate biomass for production of activated carbon at high temperatures (usually above 700 °C). At typical pyrolysis temperatures, CO 2 might also involve in biomass pyrolysis , which was investigated via pyrolysis of lignin at temperatures from 400 to 700 °C in N 2 and CO 2 atomsphere, respectively. The results suggested that CO 2 interfered with the pyrolysis process, facilitating formation of bio-oil and biochar but not gases via suppressing further gasification of volatiles. This reserved more mono-ring phenolics in bio-oil and also formed more heavier phenolics through secondary condensation routes. As for biochar, CO 2 enhanced the aromatization process, generating the carbon-rich biochar of higher heating value . The in-situ characterization of the functionalities of biochar during pyrolysis suggested that CO 2 accelerated removal of the aliphatics like -OH, -C-H, C O, and C-O-C. This rendered the biochar of hydrophobic surface but less fragmentized structures than that obtained in N 2 .
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JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Feihan Yu,Wenxuan Wang,Yudong Li,Minshu Du,Feng Liu,Daxin Liang
TiO 2 is one of the most ideal photocatalytic materials, but its application is limited by many problems (e.g., wide band gap, easy carrier recombination). Co-catalyst with changes in valence could efficiently overcome the disadvantages above. Herein, a Fe species (Fe, Fe 2 O 3 )/TiO 2 was designed to fully utilize photogenerated charges and holes. The degradation rate of ciprofloxacin can reach 99.97%. In addition, its methane generation from photoreduction of CO 2 is 12.9 times than that of pure TiO 2 . These results are attributed to the well-designed catalyst including the combination of TiO 2 and FeO x as photocatalysts and oxygen buffers, and the dispersion of single-atom Fe clusters as cocatalysts and electron trap sites. The effect mechanism of Fe species on TiO 2 was verified by PBE DFT calculation. Finally, following a concept of thermodynamic-kinetic synergy, a new design strategy for photocatalysts is accordingly proposed, as such, the prepared catalyst is expected to be applied in the environmental remediation.
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CATALYSIS COMMUNICATIONS
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2022
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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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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Hongbo Xue,Congcong Yin,Sen Xiong,Jingying Yang,Yong Wang
Solar energy-driven reduction of CO2 into fuels with H2O as a sacrificial agent is a challenging but desirable subject in photosynthesis. Covalent organic frameworks (COFs) are considered promising candidates for this subject because of their designable structures and functions. The coordination of transition metal ions into COFs is a feasible way to boost the photocatalytic activity. However, postsynthetic modification of COFs with metal ions often leads to a significant decrease in crystallinity and the specific surface area. Herein, we develop a one-pot synthesis of metal-coordinated (nonnoble metal) COFs with high crystallinity. HB-TAPT + Co with ordered and segregated D–A arrays is synthesized by combining 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT, a strong electron-acceptor) with 2-hydroxy-1,3,5-benzenetricarbaldehyde (HB)-loaded Co2+ (a strong electron-donor). The CO production when using HB-TAPT + Co under visible light irradiation for 4 h is 78.4 μmol g–1, which is 3.2 times that of HB-TAPT + Co synthesized by the postsynthetic modification method and 2.65 times that of HB-TAPT without the metal ions. HB-TAPT + Co also has good recycling stability in photocatalytic CO2 reduction. Additionally, experimental results have demonstrated that the crystallinities of these metal-coordinated materials contribute greatly to the conversion of CO2 in the photoreaction with H2O. This work provides a new protocol for improving the CO2 photoreduction performance by coordinating metal ions to COFs while maintaining the original crystallinity through a one-pot synthesis method.
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PubMed
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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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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BIOCHEMICAL ENGINEERING JOURNAL
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2022
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IF 4.446
Jiabao Xv,Zeyang Zhang,Saizhao Pang,Jiahui Jia,Zixin Geng,Ruirui Wang,Peikun Li,Muhammad Bilal,Jiandong Cui,Shiru Jia
Immobilized carbonic anhydrase (CA, EC4.2.1.1) for CO 2 capture has been intensively investigated. Unfortunately, the immobilized CA usually shows low CO 2 capture efficiency due to lack of CO 2 capture function for the conventional CA supports. In this study, an acid-resistant metal-organic framework MOF-808 was first modified by co-deposition of PEI (polyethyleneimine) and PDA (polydopamine) (PEI/PDA-MOF-808). Subsequently, the PEI/PDA-MOF-808 with a large number of amino groups was used as the strengthening material of CO 2 capture to immobilize CA (CA@PEI/PDA-MOF-808). The resultant CA@PEI/PDA-MOF-808 showed a considerably improved CO 2 capture capacity compared with free CA and PEI/PDA-MOF-808. The amount of CaCO 3 produced by CA@PEI/PDA-MOF-808 was 11.0-fold and 2.5-fold higher than free CA and PEI/PDA-MOF-808, respectively. After 8 consecutive rounds of CO 2 conversion, the total production of CaCO 3 by CA@PEI/PDA-MOF-808 was 92-fold higher than free CA, reaching 294.0 mg. Furthermore, CA@PEI/PDA-MOF-808 displayed high thermostability , pH stability, storage stability, and reusability compared with free counterpart. After 1 h treatment at pH 3.0, CA@PEI/PDA-MOF-808 preserved 53.6% of its original activity while free CA was almost inactivated. In conclusion, this work provides a promising strategy for enzymatic CO 2 conversion.
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Journal of CO2 Utilization
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2022
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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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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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Nature Catalysis
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2022
·Vol. 5
·期 6
·564-570
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IF 40.706
Xie Yi,Ou Pengfei,Wang Xue,Xu Zhanyou,Li Yuguang C.,Wang Ziyun,Huang Jianan Erick,Wicks Joshua,McCallum Christopher,Wang Ning,Wang Yuhang,Chen Tianxiang,Lo Benedict T. W.,Sinton David,Yu Jimmy C.,Wang Ying,Sargent Edward H.
Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+ ) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1 , with the lowest ∆ G OCCOH* and ∆ G OCCOH* - ∆ G CHO* . We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2 , simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+ .
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Journal of CO2 Utilization
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2022
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IF 8.321
Yuanping Zhang,Hongguang Liang,Xiaoyun Li,Qifeng Li,Junwei Wang
A highly efficient melem based mesoporous metal-free catalyst with amino and hydroxyl groups was successfully developed by template method with melamine as precursor and nano-SiO 2 as template. In the absence of any co-catalyst and solvent, the catalyst mp-CN-450 exhibits high catalytic activity for catalytic cycloaddition reaction between CO 2 and polyfunctional epoxides , and the epoxides conversion and corresponding cyclic carbonates selectivity are 99.7 % and 99.5 %, respectively. And the catalyst has hardly loss of catalytic activity after being reused for four cycles. The characterization results disclose that the high catalytic activity of the catalyst is closely related to its large specific surface area, abundant mesoporous structure and synergistic effect of N species and hydroxyl groups of melem hydrates. Additionally, through the study of different N-containing compounds, it was found that the primary amine may underwent a ring-opening reaction with epoxide. But with the addition of CO 2 , amine groups prior to reacted with CO 2 to form carbamate salt , avoided the formation of by-products, thereby improved the selectivity of cyclic carbonate. Finally, based on the above research, a possible reaction mechanism for the coupling of CO 2 to epoxides was proposed.
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CHINESE JOURNAL OF POLYMER SCIENCE
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2022
·Vol. 40
·期 10
·1183-1192
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IF 3.815
Zhang Hong-Ming,Han Guang-Ping,Cheng Wan-Li,Liu Shun-Jie,Wang Xian-Hong
High solid content CO 2 -based cationic waterborne polyurethanes (CWPUs) were prepared using CO 2 -polyols as soft segment and N -methyl diethanolamine (MDEA) as hydrophilic group. The resulting stable aqueous dispersion displayed a high solid content of 52% with a low MDEA loading of 3.52 wt%. This novel structural CWPU can provide excellent adhesive strength, whose T-peel strength could reach 173.48 N/5cm, 20% higher than that of ester-based cationic waterborne polyurethane (87.55 N/5cm). The CO 2 -based CWPU film showed only 2 wt% swelling percentage after 240 min immersion in water, and no change was observed during its immersion in 5 wt% sodium hydroxide solution. The tensile strength of CO 2 -WPUs dropped slowly to 91.2% after 480 min immersion in a 5 wt% sodium hydroxide solution, whereas that of ester-based CWPUs dropped quickly to 32% after 240 min and their mechanical properties were lost after 360 min immersion. Meanwhile, the retention of the tensile strength of the CO 2 -CWPUs was 81.5% even after 720 min immersion in 10 wt% H 2 O 2 solution, while it was only ca . 38% for the ester-based CWPUs. These results indicated that the cationic CO 2 -based CWPU may be promising waterborne adhesive with outstanding ageing resistance due to its synergistic effect from carbonate and ether groups of CO 2 -polyol structure.
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