SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Chaohui He,Peng Zhang,Yong Wang,Yujuan Zhang,Tuoping Hu,Libo Li,Jinping Li
The selective removal of carbon dioxide (CO 2 ) from acetylene (C 2 H 2 ) is an important separation process in the petrochemical industry, but is challenging due to the similar physicochemical properties of the two gases. Using CO 2 -selective adsorbents that have preferential affinity for CO 2 over C 2 H 2 in pressure swing adsorption was deemed a promising separation method for the separation of CO 2 /C 2 H 2 mixtures. Herein, we report an ultramicroporous metal-organic framework, Y-bptc, to achieve efficient separation of CO 2 /C 2 H 2 through thermodynamic and kinetic synergetic effects. The unique cage-type structure interconnected by small windows exhibits high adsorption capacity for CO 2 while efficiently impeding adsorption diffusion of C 2 H 2 , which was proved by the single-component equilibrium and kinetic adsorption curves. Grand canonical Monte Carlo (GCMC) molecular calculations further show that the µ 3 -OH − of the framework have a stronger adsorption affinity for CO 2 through forming hydrogen bonds. Breakthrough experiments using Y-bptc as a CO 2 -selective adsorbent proved that high-purity C 2 H 2 (>99%) could be directly produced from one-step separation of CO 2 /C 2 H 2 (1/1, v/v) mixtures, which greatly reduced the separation process and energy consumption. In addition, the structure of Y-bptc due to the high charge density of the Y6 cluster has high stability under humid and high-temperature conditions adding to the application possibility in industry.
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ACS Catalysis
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2022
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IF 13.7
Jianli Liang,Wei Zhang,Zheyang Liu,Qianqian Song,Zhaohua Zhu,Zhiqiang Guan,Heyi Wang,Pengjun Zhang,Jing Li,Min Zhou,Chen Cao,Hui Xu,Yang Lu,Xiangmin Meng,Li Song,Po Keung Wong,Zhifeng Jiang,Chun-Sing Lee
Boron nitride (BN)-based materials, which are commonly used as metal-free catalysts for thermal catalysis and pollution degradation, have shown potential for photocatalytic reduction of CO2 into valuable carbon fuels. However, the poor performance and the insufficient explanation of the reaction mechanism of the very few reported BN-based catalysts still seriously restrict the practical development. Herein, we synthesize a hierarchical BN-like flower catalyst composed of nanofibers (∼50 nm) by combining an in situ self-assembly strategy with a self-modification method. The photocatalytic CO2-to-CO reduction rate of BN-like flowers with low B–O species content is over 3-fold than that of BN-like flowers with high B–O species content and even more than 26.7 and 7.3 times than that of bulk BN and bulk carbon nitride (CN), respectively. Notably, the performance of the as-prepared catalysts is much higher than that of the reported BN-based catalysts and nearly all the popular metal-free CN and even comparable to most metal-based catalysts. Importantly, we in-depth investigate the reasons and mechanisms for the enhancement of photocatalytic CO2 reduction activity of BN-like flowers by combining various advanced characterizations and DFT calculations. It is found that in the BN-like flowers, B atoms linked to O atoms act as active sites, and the low B–O species content is beneficial for dynamic charge transfer and *CO desorption. In addition, the catalyst also shows good stability which is verified by cycling experiments together with molecular dynamics computation. The synthesis of the metal-free BN-based catalyst and systematic theoretical investigation will be beneficial to the development of advanced catalysts for solar fuel production.
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Nano Research
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2022
·Vol. 16
·期 3
·4152-4159
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IF 10.269
Yuan Xiaoqing,Liu Ju,Qin Jingyu,Ma Weili,Liu Guangyong,Wang Yanlei,He Hongyan
Stimuli-responsive materials have important applications in chemistry and chemical engineering. Here, we synthesized five different polyetheramine-fatty acids (PEFA) ionic liquids (ILs), possessing the dual stimuli-responsive ability to temperature and CO 2 . These PEFA ILs have reversible lower critical solution temperature (LCST) phase behavior over a wide temperature range of 37–91 °C, and reversible heterogeneous-homogeneous phase transition towards the addition and removal of CO 2 . Furthermore, the droplet size of the IL—water mixture system increased from 6.5 to 21.0 nm as the temperature increased from 25 to 56 °C, and then recovered to 6.5 nm when the temperature decreased to 25 °C. The addition and removal of CO 2 also reversibly modulated the droplet size of the system. Results from nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectra further showed that the temperature-dependent conformation of polyether amine chain in the cation dominates the temperature response, while the reversible formation of bicarbonate and fatty acids (FA) from CO 2 and anion controls the CO 2 -based reversible phase transition. Molecular simulations revealed a microscopic response mechanism of the IL—water system to temperature and CO 2 , and a synergistic effect between the dual stimuli of temperature and CO 2 . These findings may provide a basis for the rational design and understanding of ILs-based stimuli-responsive materials and nanoreactors.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Xinran Li,Shuohan Li,Jian Xu,Lanxin Wang,Kaiwei Liang,Huihui Zhang,Xuelian Yu,Zhongwei Liu
Photoconversion of CO 2 into fuel is critical for realizing a net-zero emission future, but it remains an open challenge due to the unsatisfactory light absorption and photogenerated carriers’ separation efficiency of catalysts. In this work, upon in situ thermal polymerization method, the nanodiamond (ND) are homogeneously and solidly modified on the defective graphitic carbon nitride (g-C 3 N 4 ) surface. Under visible light irradiation, the ND/g-C 3 N 4 (NH) exhibits excellent CO 2 photocatalytic performance with a CO yield of 10.98 μmol/h (18.6 times higher than bulk g-C 3 N 4 ), predominant performance in the selectivity of CO and cyclic stability. The improved CO 2 photoreduction ability was sourced from the synergetic effect of nitrogen vacancies engineering and ND decoration, which also significantly improved visible light absorption capacity and facilitated electron transport pathways, and promoted the separation and transfer of charge carriers efficiently.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Rui Li,Jenaidullah Batur,He Bian,Ying-Jie Wang,Zunbin Duan,Yabo Xie,Jian-Rong Li
Photocatalyzed CO2 reduction (CO2RR) transfers CO2 into valuable products using renewable energy, attracting widespread attention. Composite catalysts fabricated with TiO2 and red phosphorus (RP) might exhibit competitive advantages, but effective interphase binding is difficult to forge. The composites therefore require complex and energy-consuming syntheses, severely hindering their application in CO2RR. In this work, TiO2/RP composites with hyperefficient interphase contact, which outperform various elaborately designed catalysts, are directly prepared from commercially available materials via a green and facile hydrothermal approach. The low heating temperature and sole solvent of water diminish the energy input for synthesis and imply a potential opportunity to propel CO2RR with industrial waste heat and cooling water. Experimental and computational analyses reveal that hydrothermal synthesis reduces the interfering oxidized species on the exterior surface of RP, facilitating the relatively less favored interphase contact between TiO2 and nonoxidized RP. Photoelectron transfer and catalytic performance of the composites are hence drastically enhanced. Further improvement of activity is feasible by slightly elevating the heating temperature, time, or solution acidity. Attributing to the universal applicability of this green approach, different metal oxide/RP composites (e.g., WO3/RP) are similarly prepared, consistently boosting the reaction rate multiple times.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Chao Meng,Guofeng Zhao,Xue-Rong Shi,Qiang Nie,Ye Liu,Yong Lu
Carbon neutrality is spurring worldwide impetus on the exploration of CO 2 hydrogenation to methanol, but groundbreaking catalyst presents a grand challenge. An outstanding InNi 3 C 0.5 /Fe 3 O 4 catalyst is tailored by finely tuning the electronic metal-support interaction (EMSI) that is controlled by Fe 3 O 4 precursor. The one using Fe 3 O 4 - N (from ferric nitrate) stands out against the ones using Fe 3 O 4 - A (ferrous acetate) and Fe 3 O 4 - C (ferric chloride), achieving a turnover frequency (421.6 h −1 ) 2.3–3.1 times as high as that of the two others. There is a correlation between the oxygen deficiency of Fe 3 O 4 and the EMSI-governed activity. The EMSI effect is enhanced substantially by the highly oxygen-deficient Fe 3 O 4 - N . Enhanced EMSI makes InNi 3 C 0.5 electron-enriched and thus enables CO 2 to be dissociated easily. The InNi 3 C 0.5 /Fe 3 O 4 - N achieves a high methanol space time yield of 2.60 g MeOH g cat −1 h −1 with 92.0% methanol selectivity at 325 °C and 6.0 MPa. This catalyst is also highly anti-sintering and anti-sulfur poisoning.
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ACS Applied Nano Materials
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2022
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IF 6.14
Yue Liu,Xukun Zhu,Ling Qin,Tong Zhang,Shuhan Wang,Yachao Jin,Li Song,Ming-Dao Zhang
The construction of special heterogeneous interface structures without precious metals is found to be efficient for the development of low-cost and high-activity hydrogen evolution reduction (HER) catalysts. Here, we report a moderate method to develop an efficient and stable HER electrode especially composed of the Co2(OH)2CO3 (COC) nanowire substrate modified by benzenehexol (HOB) molecules. This kind of interfacial structure leads to prominent electrocatalytic HER performance in an alkaline environment with a low overpotential of 130.8 mV at a current of 20 mA cm–2. Meanwhile, density functional theory (DFT) calculations reveal that the nanoscale synergistic interfacial mechanism and strong electron interaction between HOB and COC can reduce the activation energy for HER.
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Solar RRL
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2022
·Vol. 6
·期 10
·2200536
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IF 9.173
Rui Zhang,Linjia Li,YinYin Li,Dejun Wang,Yanhong Lin,Tengfeng Xie
CsPbBr 3 perovskite exhibits potential application in photocatalytic CO 2 reduction into valuable chemical fuels; however, enhancing carrier separation capability of the CsPbBr 3 and fully understanding the CO 2 reduction reaction process are still imperative. Herein, a new series of x SnS 2 /CsPbBr 3 nanocrystals (NCs)- y heterostructures are developed, which exhibit better catalytic activity in comparison with pure CsPbBr 3 NCs. Interface and surface carrier dynamic investigation reveals that this heterojunction structure can effectively improve carrier separation efficiency. Based on the interfacial electric field direction of CsPbBr 3 to SnS 2 , it is suggested that SnS 2 /CsPbBr 3 NC heterostructure satisfies Z-scheme transfer dynamics. Meanwhile, by the aid of in situ surface photovoltage, it is experimentally confirmed there is dynamic carrier interaction between CO 2 molecules and the SnS 2 /CsPbBr 3 NCs photocatalyst under irradiation, and a photocatalytic CO 2 reduction mechanism is thus proposed. This work expands the awareness of the interaction between CO 2 and the photocatalyst, which can be strongly influenced by carrier separation efficiency at the photocatalyst heterojunction.
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JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 32
·15474-15487
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IF 4.682
Liu Jiaxin,Qi Fei,Zhang Nan,Yang Jiayu,Liang Zhiyu,Tian Changqing,Zhang Wenxia,Tang Xiaosheng,Wu Daofu,Huang Qiang
Exploring novel and efficient photocatalysts to accelerate CO 2 photoreduction into useful chemicals or fuels is of great significance. In this work, we developed the three-dimensional (3D) structural heterojunction photocatalysts composed of ReS 2 and Cu 2 O by a drop-casting approach. The ReS 2 microspheres with nanosheets were deposited on the 3D structure of Cu 2 O/Cu foams. The analysis of UV–Vis absorption and PL spectra showed that the ReS 2 @Cu 2 O/Cu heterostructure delivered enhanced visible light absorption and improved charge carrier separation. The resulting ReS 2 @Cu 2 O/Cu-180 exhibited the CO yield of 14.3 µmol g −1 under the visible light irradiation. The realized S-scheme heterostructure not only promoted the separation of the photogenerated electron and hole pairs, but also enhanced the visible light absorption. Furthermore, the enriched electrons with high reducing abilities aggregated into the conduction band and diffused to the surface of Cu 2 O for favoring the CO 2 reduction and CO formation. This study is expected to provide a strategy to prepare high-performance S-scheme photocatalysts to perform efficient photocatalytic CO 2 reduction.
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Materials Today Energy
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2022
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IF 9.257
Xinxin Bian,Bowen Liu,Xiaolei Wang,Zhimin Chen,Rui Gong,Wanqi Jia,Zichen Song,Huiyuan Meng,Weibo Yin,Zhiyu Ren
Defects engineering is one of the effective strategies to advance the CO 2 conversion into value-added chemicals and fuels during the electrochemical process. It is noteworthy that multiple defects are often associated in the reaction process, hence how to stimulate their synergistic effect is extremely important, but still lacks in-depth understanding. Herein, SnO 2 nanosheets with simultaneous oxygen vacancies and Zn dopants (Zn–Vo–SnO 2 ), as a proof-of-concept study, were proposed to elucidate the synergistic effect of multiple defects on enhanced CO 2 -to-C 1 conversion. Zn–Vo–SnO 2 , which is prepared by coupling a facile hydrothermal reaction and a subsequent desulfurization, yields the C 1 products at the lower applied potential, and maintains the FE C1 of about 95% at −0.80 V vs. RHE for a long-term operation. Evidences from systematic experiment and theoretical calculation corroborate that the charge redistribution caused by the oxygen vacancies and Zn-doping synergistically energize the CO 2 conversion, in the term of the CO 2 adsorption, the hydrogenation of CO 2 and intermediates, and the thermodynamic energies of the rate-determining steps. This study has an insight into defect engineering to design advanced electrocatalysts for implementable CO 2 recycling and utilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xinxin Han,Bingjie Lu,Xin Huang,Cheng Liu,Shixia Chen,Jingwen Chen,Zheling Zeng,Shuguang Deng,Jun Wang
S-scheme photocatalysts are more efficient than the conventional type-II configuration, but the CO 2 reduction performances are still unsatisfactory. Herein, we firstly report the layered double hydroxide (LDH) based S-scheme heterostructure photocatalyst (NiIn LDH/In 2 S 3 ) with n-type NiIn LDH and p-type In 2 S 3 . The built-in internal electric field directs the photogenerated electrons flow from the conductive band of In 2 S 3 to the valance band of NiIn LDH, which is confirmed by operando and theoretical experiments. The CO 2 photoreduction intermediates are monitored by in-situ Raman spectra, and the density functional calculations disclose the reduced energy barrier for CO desorption on the heterojunction. Therefore, without cocatalysts or sacrificial agents, the NiIn LDH/In 2 S 3 heterojunction delivers a high CO yield rate of 29.43 μmol g −1 h −1 under visible light irradiation, ca. 3.5 and 4.3 times higher than the single counterpart NiIn LDH and In 2 S 3 . Notably, this value is the highest among S-scheme CO 2 photocatalysts and surpasses most top-ranking benchmarks.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Cuihua Ma,Qinghua Li,Zhi Wang,Min Gao,Jixiao Wang,Xingzhong Cao
Polymeric membranes have been widely researched for several decades due to their good processability and low cost. Herein, high-performance thin-film composite (TFC) membranes were prepared by interfacial polymerization using N-methyldiethanolamine (MEDA), 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethylspirobisindane (TTSBI) and trimesoylchloride (TMC). The effects of segmental chain motion on the gas separation performance of the TFC membranes were investigated for the polymeric membranes featuring rigid and contorted sites along the polymer backbone by inducting TTSBI. The results suggested that the introduction of rigid and contorted structures improved the cavities in the membrane, impeded the transport of larger gas, and enhanced the diffusive selectivity. Therefore, the TFC membrane exhibited high permeance and high selectivity with CO 2 permeance of about 1800 GPU and CO 2 /N 2 selectivity of 370 at 0.11 MPa, which is a remarkable improvement in gas separation performance.
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