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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Superhydrophobic UHMWPE Foams with High Mechanical Robustness and Durability Fabricated by Supercritical CO2 Foaming

Binbin Sun,Jun Li,Yahao Guo,Heng Li,Hao-Yang Mi,Binbin Dong,Chuntai Liu,Changyu Shen

The low durability and stability of superhydrophobic foams and high fabrication costs are the main reasons that limit their practical applications in water remediation and oil recycling. Herein, an extremely superhydrophobic and exceptionally robust foam was developed based on ultrahigh-molecular weight polyethylene (UHMWPE) by supercritical carbon dioxide (scCO2) foaming and subsequent surface modification. The developed foam comprises a highly porous structure decorated with hydrophobic silica nanoparticles and aligned UHMWPE crystallites, constructing a complex micro–nanosized hierarchical morphology, which contributed to an unprecedented water contact angle (WCA) of 162° and a sliding angle of 1°. When used in selective oil absorption and oil/water separation, the foam demonstrated about 100% separation efficiency in repetitive use and even under a vacuum of −70 Kpa due to its high water repellency. More importantly, the foam has outstanding tolerance against mechanical damages such as ultrasonication, bending and twisting, tape peeling, steel wool abrasion, and knife scratching. The surface could maintain the hierarchical structure and a WCA of over 156° after enduring different damages. Moreover, when the surface is clogged, the foam could restore its superhydrophobicity by arbitrary fracturing and cutting, resulting in a theoretically unlimited lifespan. This work not only proposes a UHMWPE-based superhydrophobic foam with extremely high superhydrophobicity, durability, and separation efficiency but also provides insights into the design and mass production of ultraefficient and robust superhydrophobic porous materials for practical applications.

CAS / MDL: 7631-86-9
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Molecular Catalysis · 2021 · IF 5.062

Facile synthesis of carboxyl- and hydroxyl‑functional carbon nitride catalyst for efficient CO2 cycloaddition

Xin Wang,Lei Shi,Yanglin Chen,Chaokun Yang,Li Yang,Jianmin Sun

With the aim of green chemistry and sustainable development, the coupling of CO 2 with epoxides to cyclic carbonate is an attractive and promising CO 2 fixation without byproducts. Solvent- and metal-free heterogeneous catalysts offer an environmentally friendly and convenient separation alternative to traditional metal-based or homogeneous catalysts. Hence, hydrolyzed carbon nitride (HCN) was successfully synthesized via urea-derived carbon nitride (CN) hydrolyzed in NaOH solution and the freeze-drying (FD) method was adopted to obtain the HCN-FD catalyst. The composition and chemical properties of HCN-FD were thoroughly characterized by different analysis methods. The synergistic effects of hydrogen-bond donors of –COOH, –OH and –NH X in HCN-FD resulted in improved acidity sites characterized by NH 3 -TPD. Compared with CN, HCN-FD combined with tetrabutylammonium iodide cocatalyst displayed satisfactory catalytic performance in the CO 2 cycloaddition due to more exposed active sites (–COOH, –OH and –NH X ). Moreover, the recyclability and versatility of the HCN-FD catalyst were excellent in CO 2 cycloaddition reaction. Thus, the HCN-FD catalyst was a potential candidate for the practical utilization of CO 2 fixation due to its advantage of facile synthetic method, inexpensive raw material and environmental friendliness.

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JOURNAL OF THE CHINESE CHEMICAL SOCIETY · 2021 ·Vol. 69 ·期 2 ·289-300 · IF 1.967

Mixed-matrix membranes based on Li1.6Mn1.6O4 (LMO) ultrathin nanosheet for high-performance CO2 separation

Fu Liu,Weifang Zhu,Minmin Gou,Hengheng Cao,Ruili Guo

Two-dimensional flake Li 1.6 Mn 1.6 O 4 (LMO) was added to the Pebax®MH 1657 (Pebax) matrix to prepare mixed-matrix membranes (MMMs) for CO 2 /CH 4 mixed gas separation. The average pore diameter of the LMO nanosheet was about 10.79 nm: a fast CO 2 transport channel could be established in the membrane. In addition, the Li and oxygen defect site (O δ− ) in the LMO had an affinity for CO 2 , which improved the permeability of the membrane and the selectivity for CO 2 separation. Furthermore, the ultrathin structure of LMO with large aspect ratio was also conducive to gas separation. When the LMO filling amount was 2.0 wt%, the permeation rate of pure CO 2 gas of Pebax/LMO-2.0 membrane was 117.9 Barrer, and the CO 2 /CH 4 ideal selectivity was 18.74, which were 119.7 and 35.8% higher than Pebax membrane, respectively. The CO 2 /CH 4 mixed gas separation results of Pebax/LMO-2.0 membrane showed that the CO 2 permeability and CO 2 /CH 4 selectivity were 158.54 Barrer and 33.41, respectively, and were increased by 83.24 and 23.15%, compared with Pebax membrane.

CAS / MDL: 1310-65-2
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DALTON TRANSACTIONS · 2021 ·Vol. 50 ·期 45 ·16711-16719 · IF 4.39

Immobilizing CsPbBr3 perovskite nanocrystals on nanoporous carbon powder for visible-light-driven CO2 photoreduction

Ying Jiang,Cunxin Mei,Zhijie Zhang,Zhongliang Dong

Perovskite CsPbBr3 nanocrystals (NCs) have emerged as promising candidates for the photocatalytic reduction of CO2. However, the CO2 conversion efficiency of pristine CsPbBr3 is still unsatisfactory, mainly due to severe radiative recombination, poor stability and low CO2 capturing ability. Coincidentally, nanoporous carbon powder (NCP) has received tremendous attention for environmental remediation and renewable energy production. Herein, by immobilizing CsPbBr3 NCs into the pores of NCP, a CsPbBr3/NCP hybrid has been successfully constructed for the first time, which combined the advantages of CsPbBr3 NCs and NCP. In comparison with pristine CsPbBr3, the resultant hybrid photocatalyst exhibited much superior photocatalytic performance in CO2 reduction, which could be attributed to the enhanced electron extraction and transfer between CsPbBr3 NCs and NCP, higher CO2 capturing ability and more active sites for CO2 activation. Furthermore, the nanohybrid displayed remarkable reusability in photocatalytic CO2 reduction. This study is anticipated to provide a new pathway for the design and fabrication of high-performance photocatalysts based on perovskites for solar-energy-conversion applications.

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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Sustainable separation of petroleum hydrocarbons pollutant using hydrophobic deep eutectic solvents regulated by CO2

Xiaojiang Li,Leitao Sun,Xin Lv,Jie Qi,Hongsheng Lu,Yuanpeng Wu,Baogang wang

Petroleum hydrocarbons pollutants are the serious environmental hazards in the exploitation of petroleum resources. As comparison to the traditional solvent for petroleum hydrocarbons removal, deep eutectic solvents (DESs), as the ideal alternate for organic solvents, have non-toxicity, non-flammability and lower volatility. Whereas, the recycling of DES is still the great challenge for sustainable separation. Herein, hydrophobic DESs (HDESs) with the CO 2 switchable-hydrophilicity are developed, aiming to sustainably separate petroleum hydrocarbons pollutions. The HDESs are formed by hydrogen bonds between the phenolic compounds as hydrogen bond donors (HBDs) and tertiary amines as hydrogen bond acceptors (HBAs), which was demonstrated by the spectroscopic detection. Interestingly, the HDES exhibits better CO 2 -switchable behavior than traditional switchable-solvent, where the phase transition is induced by the protonation of HBA upon CO 2 and the deprotonation of HBD in HCO 3 - solution of HBA. Furthermore, the sustainable separation for oils (heptane, diesel oil and crude oil) is successfully completed, and the HDES is also easily recovered upon N 2 /65 °C. Finally, the HDES is effectively applied in removing petroleum hydrocarbons from oily wastes (oil sands and oily sludge). The results show that more than 98% oil is removed from oil sands, and 85.02% oil is also removed from oily sludge . Thus, the HDESs will be expected to treated as the effective extractant for sustainable and cleaner separation of petroleum hydrocarbons- contaminated waste.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Efficient-and-stable CH4 reforming with integrated CO2 capture and utilization using Li4SiO4 sorbent

Zongze Lv,Changlei Qin,Shuzhen Chen,Dawid P. Hanak,Chunfei Wu

CO 2 capture and utilization has been considered as an up-and-coming short- to mid-term approach to mitigate the excessive CO 2 emission. Comparing to the conventional separate capture, transportation and conversion arrangement, the integrated CO 2 capture and utilization (ICCU) could largely simplify the complex process and reduce the energy consumption. However, the poor stability of high-temperature CO 2 sorption/desorption severely limit the potential of ICCU. Therefore, it is indispensable to develop a new sorbent/catalyst system ensuring the high-efficiency and long-term operation of the ICCU. In this paper, we propose and demonstrate the feasibility and performance of using K 2 CO 3 -doped Li 4 SiO 4 as an efficient CO 2 sorbent for ICCU operating at a relatively low temperature by dry reforming of methane. Results show that the ratio of H 2 /CO produced is stabilized at 1 ± 0.05 in the pre-breakthrough stage, and the duration extends to be 1.6 times of the original value in the cyclic operations, displaying an excellent performance in reaction matching and process stability.

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ACS Applied Energy Materials · 2021 · IF 6.024

Low-Pressure CO2 Capture in Zeolite Imidazole Frameworks with Ultramicropores Studied by Positron Annihilation

Mengde Li,Junjie Liu,Shuping Deng,Qian Liu,Ning Qi,Zhiquan Chen

In this paper, three kinds of zeolite imidazole frameworks (ZIF-90, ZIF-93, and ZIF-94) were synthesized through hydrothermal reactions. Positron lifetime results reveal two kinds of pores corresponding to the channel in the windows and central cavity of ZIFs. The average diameters of the cavities are 1.12, 1.54, and 0.80 nm in ZIF-90, ZIF-93, and ZIF-94, respectively, while the average diameters of channels are between 0.55 and 0.60 nm. CO2 adsorption results show that ZIF-90 has the highest CO2 adsorption capacities (64.4 cm3 g–1 at 298 K and 104.7 cm3 g–1 at 273 K) at 1 bar, followed by ZIF-94 (57.9 cm3 g–1 at 298 K and 79.4 cm3 g–1 at 273 K) and ZIF-93 (41.5 cm3 g–1 at 298 K and 62.5 cm3 g–1 at 273 K). This shows inconsistency with the total pore volume but is in good agreement with relative volumes of pores smaller than 1.2 nm, which are 6.55, 2.06, and 5.60% for ZIF-90, ZIF-93, and ZIF-94, respectively. Further investigation reveals that an even smaller pore size is required for CO2 adsorption under ultralow pressure. At a pressure of 0.1 bar, ZIF-94 exhibits an ultrahigh CO2 adsorption capacity (21.2 cm3 g–1 at 298 K and 32.1 cm3 g–1 at 273 K) compared with ZIF-93 (10.1 cm3 g–1 at 298 K and 14.9 cm3 g–1 at 273 K) and ZIF-90 (5.9 cm3 g–1 at 298 K and 11.6 cm3 g–1 at 273 K). These quantities coincide well with the relative volumes of pores smaller than 0.8 nm, which are 5.60, 2.06, and 1.18% for ZIF-94, ZIF-93, and ZIF-90, respectively. Our results demonstrate that at atmospheric pressure, CO2 molecules are more effectively captured by micropores, while at extremely low pressures, CO2 molecules are mainly enriched around ultramicropores such as the channels and small cavities in ZIFs.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Enhancing efficiency of perovskite solar cells from surface passivation of Co2+ doped CuGaO2 nanocrystals

Ruoshui Li,Yanfei Dou,Yinsheng Liao,Deng Wang,Guodong Li,Jihuai Wu,Zhang Lan

Before completely applying inorganic materials as hole transport materials (HTM) for perovskite solar cells (PSCs), modifying devices with inorganic oxides that have the potential as inorganic hole transporters is an effective way to improve device performance and stability. Co 2+ doped CuGaO 2 nanocrystals (Co-CuGaO 2 NCs) with sizes about 20 nm are synthesized by hydrothermal method and used for surface passivation at the interface of perovskite (PVK)/2,2′,7,7′-Tetrakis[ N , N - di (4- methoxyphenyl ) amino ]-9,9′-spirobifluorene (spiroOMeTAD). Co-CuGaO 2 NCs have a larger bandgap with lower valance band compared with spiroOMeTAD, which is more beneficial to the conduction of holes and the blocking of electrons. Furthermore, the Co-CuGaO 2 has a lower valance band energy compared with the original CuGaO 2 , which reduces the energy gap between Co-CuGaO 2 and PVK. Co-CuGaO 2 NCs fully cover the upper surface of PVK, which helps prevent direct contact between PVK and oxygen and moisture. The Co-CuGaO 2 NCs surface passivation also gives better hole transport as revealed by the ultraviolet photoelectron spectroscopy (UPS), steady-state photoluminescence (PL), and time-resolved photoluminescence (TRPL) data. When the concentration of Co-CuGaO 2 NCs solution is set to 7.5 mg mL −1 , the device exhibits a best PCE of 20.39% and maintains 84.34% of the initial power conversion efficiency (PCE) after stored 30 days under air atmosphere with 15 ± 5% humidity.

CAS / MDL: 34819-78-8
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Conversion of CO2 to formic acid by integrated all-solar-driven artificial photosynthetic system

Jiwu Zhao,Lan Xue,Zhenjie Niu,Liang Huang,Yidong Hou,Zizhong Zhang,Rusheng Yuan,Zhengxin Ding,Xianzhi Fu,Xu Lu,Jinlin Long

Sunlight-driven valorization of CO 2 into fuels is a promising solution to renewable energy storage , but the design of an integrated and efficient solar-to-chemical conversion system remains challenging. Herein, an all-solar-driven artificial photosynthetic system (APS) by tailoring photovoltaic-photoelectrochemical cell which can efficiently produce formic acid fuel from CO 2 and H 2 O with bias-free illumination is demonstrated. Guided by density functional theory (DFT) calculations, a BiOI–Bi (BOI–Bi) cathode catalyst is synthesized, which is highly selective for CO 2 to HCOOH conversion, and coupled with a single crystalline argon-treated TiO 2 (TiO 2 -Ar) photoanode, whose valence band edge is beneficial for the oxidation of H 2 O to O 2 . The APS exhibits high product selectivity, robust activity and good durability. A solar-to-HCOOH selectivity of 96.5% is obtained with a HCOOH yield of 108.2 mmol g −1  h −1 under bias-free illumination of AM1.5G. The device can operate stably for at least 12 h. In particular, an apparent photon quantum efficiency of 7.5% and a solar-to-chemical conversion efficiency (η SCC ) of 8.3% are recorded, rivaling all the incumbent precious-metal-free all-solar-driven components for CO 2 -to-HCOOH conversion. This study highlights the potential of BOI-Bi for CO 2 to HCOOH conversion with high selectivity and its integration into APS system to realize carbon-negative solar-to-chemical conversion with industrial relevance.

CAS / MDL: 7440-69-9
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JOURNAL OF CATALYSIS · 2021 · IF 7.92

Morphology-engineered highly active and stable Pd/TiO2 catalysts for CO2 hydrogenation into formate

Jing Zhang,Weiqi Liao,Hao Zheng,Yunshang Zhang,Lebing Xia,Bo-Tao Teng,Ji-Qing Lu,Weixin Huang,Zhenhua Zhang

Pd supported on different anatase TiO 2 nanocrystals predominantly exposing either {1   0   0}, {1   0   1}, or {0   0   1} facets were tested for CO 2 hydrogenation into formate. Remarkable morphology-dependent catalysis was observed. Compared to 2%Pd/TiO 2 {1   0   1} and 2%Pd/TiO 2 {0   0   1} catalysts, 2%Pd/TiO 2 {1   0   0} is highly active and stable, affording an unprecedented turnover frequency of ca. 1369 h −1 and keeping stable after 6 cycles at 313 K. This can be associated with, on the one hand, higher density of moderate basic site and relatively more Pd(0) species over 2%Pd/TiO 2 {1   0   0} contribute to the activations of CO 2 and H 2 , respectively, favorable for the activity; On the other hand, higher oxygen vacancy concentrations in the TiO 2 {1   0   0} promote the Pd-TiO 2 interactions and result in the formation and stability of flat Pd particles over 2%Pd/TiO 2 {1   0   0}, beneficial to the stability. These results highlight the importance of oxide morphology in formate formation and open up possibilities of oxide morphology engineering for developing efficient Pd-based catalysts for CO 2 hydrogenation.

CAS / MDL: 13463-67-7
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APPLIED CLAY SCIENCE · 2021 · IF 5.467

Encapsulated Lewis acidic ionic liquids by halloysite using as efficient catalyst for CO2 conversion

Jiangtao Peng,Haowei Sun,Jian Wang,Peiping Zhang,Weikun Ning,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Shiding Miao

A type of clay-supported catalysts were developed for conversion of CO 2 by encapsulating ZnBr 2 -based Lewis acidic ionic liquids (ZnBr 2 /IL) in halloysite (Hal) via a one-step strategy. The Lewis acidic ionic liquid was loaded within enlarged lumens of Hal via acid treatment, and the mesoporous structure was found to benefit for CO 2 storage/conversion. The composite ZnBr 2 /IL@P-Hal was found to have an adsorption capacity (6.43 cm 3 /g) of CO 2 via adsorption/desorption isotherm measurements. The composite ZnBr 2 /IL@P-Hal showed excellent catalytic performance (TOF value was 1747.7 h −1 ) for coupling of CO 2 with epoxides to produce propylene carbonate under the lack of any cocatalyst . Kinetic investigations indicated the reaction followed an order of one, with respect to catalyst ZnBr 2 /IL@P-Hal. The overall pathway of CO 2 cycloaddition was theoretically validated via DFT calculations. These experimental and computational efforts deepen comprehension of the rational design of clay-based catalysts for CO 2 cycloaddition, further elucidated halloysite was a promising support.

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Sustainable Energy & Fuels · 2021 ·Vol. 5 ·期 24 ·6449-6459 · IF 6.367

High-performance Ni–Ce1−xZrxO2 nanoparticles for biogas reforming: enhanced CO2 activation and stability

Zhige Zhang,Guofeng Zhao,Han Bing,Jiawei Zhong,Haoran Yuan,Jun Xie,Yong Chen

The efficient utilization of renewable biogas has attracted ever-increasing interest in the past few decades. Ni–Ce1−xZrxO2 supported on monolithic SiC-F (named Ni–Ce1−xZrxO2/SiC-F) is developed and applied in biogas reforming. Monolithic Ni–Ce1−xZrxO2/SiC-F catalysts were comprehensively characterized by ICP-AES, XRD, SEM, HR-TEM, CO2-TPD, etc. The promotional roles of Ce1−xZrxO2 in coke elimination as well as CO2 activation were deeply analyzed via in situ CH4-TPSR/CO2-TPO and in situ H2-TPR/CO2-TPSR. Ni–Ce1−xZrxO2/SiC-F exhibits satisfactory catalytic activity and ability to inhibit sintering and coke-deposition due to (a) the homogeneous dispersion of Ni nanoparticles (NPs) and (b) the strong interaction between Ce1−xZrxO2 solid solutions and Ni NPs. At 900 °C and a weight hourly space velocity (WHSV) of 24 000 mL gcat−1 h−1, an excellent CH4/CO2 conversion of 90/92% was initially achieved over the Ni–Ce1−xZrxO2/SiC-F catalyst, followed by a slight decrease after 150 h, but remained basically stable for the next 250 h.

CAS / MDL: 13478-00-7
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