DALTON TRANSACTIONS
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2022
·Vol. 51
·期 20
·8036-8045
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IF 4.569
Shengqi Xu,Lu Yang,Yixuan Wei,Yiming Jia,Meiqi Hu,Lianxia Bai,Junzheng Zhang,Xinxin Li,Shuo Wei,Jun Lu
Converting CO2 into valuable solar fuels through photocatalysis has been considered a green and sustainable technology that is promising for alleviating global warming and providing energy in an environmentally friendly manner. However, traditional photocatalysts generally suffer from low surface-reactive reaction sites, inefficient light harvesting and rapid recombination of electron–hole pairs. Lead halide perovskite materials have been considered ideal semiconductor photocatalysts for photocatalytic CO2 reduction due to their tunable band gaps, strong light absorption, and low cost. Herein, a series of L2Csn−1PbnX3n+1 (L = ba, ha, oa; X = Cl, Br, I; n = 1, 2) 2D layered perovskites were synthesized by a facile solvothermal method. The effects of alkyl amine chain length, halogen atoms and inorganic layer number on their properties were studied. More importantly, these 2D materials were used as photocatalysts for CO2 reduction without any sacrificial agents. These 2D perovskites exhibited markedly increased performance in comparison with 3D bulk materials, benefitting from the larger surface-area-to-volume ratio and faster and more efficient exciton dissociation, which achieved the highest CO yield of 158.69 μmol g−1 h−1 and CH4 yield of 6.9 μmol g−1 h−1 through the design of the photocatalytic system. In addition, the influence of light source conditions on photocatalysis was studied systematically, including light source intensity and wavelength. The experimental results indicated that an appropriate solvent, high light intensity and monochromatic light source matching the wavelength of exciton absorption can effectively improve the photocatalytic efficiency.
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CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Linlin Wang,Xin Li,Leiduan Hao,Song Hong,Alex W. Robertson,Zhenyu Sun
To facilitate the electrochemical CO 2 reduction (ECR) to fuels and valuable chemicals, the development of active, low cost, and selective catalysts is crucial. We report a novel ECR catalyst consisting of CuO nanoparticles with sizes ranging from 1.4 to 3.3 nm anchored on Cu metal-organic framework (Cu-MOF) nanosheets obtained through a one-step facile solvothermal method. The nanocomposites provide multiple sites for efficient ambient ECR, delivering an average C 2 H 4 faradaic efficiency (FE) of ~50.0% at –1.1 V (referred to the reversible hydrogen electrode) in 0.1 mol/L aqueous KHCO 3 using a two-compartment cell, in stark contrast to a C 2 H 4 FE of 25.5% and 37.6% over individual CuO and Cu-MOF respectively, also surpassing most newly reported Cu-based materials under similar cathodic voltages. The C 2 H 4 FE remains at over 45.0% even after 10.0 h of successive polarization. Also, a ~7.0 mA cm −2 C 2 H 4 partial geometric current density and 27.7% half-cell C 2 H 4 power conversion efficiency are achieved. The good electrocatalytic performance can be attributed to the interface between CuO and Cu-MOF, with accessible metallic moieties and the unique two-dimensional structure of the Cu-MOF enhancing the adsorption and activation of CO 2 molecules. This finding offers a simple avenue to upgrading CO 2 to value-added hydrocarbons by rational design of MOF-based composites.
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ACS Catalysis
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2022
·
IF 13.7
Shuangxi Lin,Qiang Wang,Maoshuai Li,Ziwen Hao,Yutong Pan,Xiaoyu Han,Xiao Chang,Shouying Huang,Zhenhua Li,Xinbin Ma
Controlling the selectivity of CO2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO2 hydrogenation. The alloying of Ni with Zn to charged (Niσ––Znσ+) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H2, and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO2 species in a η2(C, O) bridge configuration, directly dissociate the C═O bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.
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ENERGY & FUELS
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2022
·
IF 4.654
Zhijun Zhao,Jubao Gao,Mingsheng Luo,Xinyue Liu,Yongsheng Zhao,Weiyang Fei
In recent decades, ionic liquids (ILs) have been developed as an ideal and reversible decarbonization solvent. However, some pitfalls, such as the low CO2 capacity and high viscosity of ILs, limit their further scale up and industrial application. Therefore, in this work, three novel functional ILs [N8881][NIA], [N8881][For], and [N8881][Ac] were synthesized after using a molecular design method to capture CO2 at 303.15–333.15 K and pressures up to 1000 kPa. The experimental results illustrate that [N8881][NIA] presents the smallest viscosity and the highest CO2 solubility. The capacity order is [N8881][NIA] > [N8881][For] > [N8881][Ac] under the same experimental conditions. The CO2 recyclability experiments using [N8881][NIA] show the stability of CO2 solubility after 5 cycles. The quantum chemistry simulations at the level of DFT/B3LYP with 6-311++G(d,p) basis sets were used to study the CO2 absorption mechanism in the studied ILs from the molecular viewpoint. Simulation results illustrated that the higher interaction energy between CO2 and ILs means more CO2 absorbed in these ILs, which agreed well with the experimental results. The atoms in molecules theory and the function of the reduced density gradient were also used to calculate the interactions in these IL–CO2 systems. Results show that the majority of these interactions present an electrostatic character.
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Biomass Conversion and Biorefinery
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2022
·Vol. 13
·期 15
·14049-14058
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IF 4.05
Yan Mi,Zhang Yan,Grisdanurak Nurak,Wibowo Haryo,Yu Caimeng,Kanchanatip Ekkachai
One outstanding advantage of supercritical water gasification (SCWG) coupled with CO 2 capture and storage (CCS) technology is to realize the conversion of bio-waste into hydrogen-rich syngas. In this study, metal organic frameworks of copper benzene-1,3,5-tricarboxylate (Cu-BTC) were synthesized via solvothermal method with different synthesis time and used as adsorbent for capturing CO 2 from SCWG model syngas. The effect of synthesis time, adsorption temperature, and adsorption pressure on CO 2 adsorption capacity of Cu-BTC was evaluated using analysis of variance (ANOVA). The Pareto chart showed that adsorption pressure had significant effect on CO 2 adsorption capacity, and the surface plot indicated that CO 2 adsorption capacity increased with higher adsorption pressure and lower adsorption temperature. Cu-BTC with 48-h synthesis time had the largest specific surface area (1737 cm 2 /g) and pore volume (0.73 cm 3 /g), and it exhibited the highest CO 2 capacity of 19.83 mmol/g and 13.56 mmol/g at 0 °C and 25 °C, respectively. The adsorption results showed that CO 2 concentration in multi-component gas decreased from 48.75 to 12.9%, and H 2 concentration increased from 38.75 to 75.45%. Therefore, Cu-BTC has the potential for removal of CO 2 from SCWG syngas, and more work is necessary to further improve the adsorption capacity and selectivity. Graphical abstract
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Wenchao Zheng,Zuyi Yan,Rui Zhang,Wusan Jiang,Xiao Luo,Zhiwu Liang,Qi Yang,Hai Yu
The kinetics between BZA and CO 2 were investigated by the stopped-flow apparatus over the BZA concentration range from 0.05 to 0.1 mol/L (0.54–1.07 mass%), and over the temperature range from 293 to 313 K. The results also show that the predicted CO 2 absorption rate exhibits good agreement with the experimental data with an absolute average deviation (AAD) of 5.15% and 4.15% with respect to the zwitterion and termolecular models, respectively. Furthermore, the NMR experiments confirmed the formation of carbamates. The VLE plots were made with speciation data obtained from NMR techniques applied to the CO 2 -BZA-H 2 O system with CO 2 loading of 0–0.67 mol CO 2 /mol BZA at 298 K. A new VLE model was proposed, and the predicted results exhibit good agreement with the experimentaly measured results.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 27
·e52485
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IF 3.057
Xiaoshuai Zhu,Xijue Li,Hao-Yang Mi,Xin Jing,Binbin Dong,Ping He,Chuntai Liu,Changyu Shen
Thermoplastic polyurethane (TPU) foams are commonly used buffering materials due to their lightweight, high elasticity, and excellent energy absorption properties. Improving their compressive property without increase foam density is a challenge for TPU foams. Herein, graphene oxide (GO)/TPU composite foams containing micro-sized wrinkles on the cell surface were fabricated by a novel dynamic supercritical carbon dioxide (scCO 2 ) foaming method. The addition of GO created hydrogen bonding and physical crosslinking sites with the TPU molecules, which acted as nucleation agents to improve the cell density of the GO/TPU foams. With the increase of GO content, the mechanical properties of GO/TPU foams were significantly enhanced, and the wrinkled foams prepared via dynamic scCO 2 foaming displayed superior compressive modulus, strength, energy absorption, and recoverability compared with the counterpart foams without wrinkly structure. The wrinkled GO/TPU foams with 0.5 wt% GO revealed higher expansion ratio, lower foam density, superior compressive property and energy absorption than both neat TPU and 1 wt% GO foams owing to the reinforcing effect of the wrinkly structure. This study is of great significance in the development of low-density composite foams with enhanced compressive performance by wrinkly structures.
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Energy & Environmental Materials
·
2022
·Vol. 6
·期 3
·e12364
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IF 13.443
Liang Lu,Chunwen Sun,Jian Hao,Zelin Wang,Sergio F. Mayer,Maria Teresa Fernández-Díaz,José Antonio Alonso,Bingsuo Zou
The recovery and utilization of carbon dioxide (CO 2 ) is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality. The Na-CO 2 battery made with cheap alkali metal sodium and greenhouse gas CO 2 is an effective strategy to consume CO 2 and store clean renewable energy. However, the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO 2 batteries. In this work, magnesium-doped Na 3 Zr 2 Si 2 PO 12 (NZSP) was studied as a solid electrolyte for solid-state Na-CO 2 batteries. The ionic conductivity of Na 3.2 Zr 1.9 Mg 0.1 Si 2 PO 12 reaches 1.16 mS cm −1 at room temperature by replacing Zr ions in Na 3 Zr 2 Si 2 PO 12 with Mg ions, and the structural changes are analyzed by neutron powder diffraction. The composite electrolyte consisting of highly conductive Na 3.2 Zr 1.9 Mg 0.1 Si 2 PO 12 and high processability poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) is utilized for the first time to assemble a solid-state Na-CO 2 battery. The cell shows a full discharge capacity of 7720 mAh g −1 at 200 mA g −1 . The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g −1 and at a cut-off capacity of 500 mAh g −1 . This work demonstrates a promising strategy to design high-performance solid-state Na-CO 2 batteries.
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ChemSusChem
·
2022
·Vol. 15
·期 14
·e202200337
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IF 9.14
Li-Qi Qiu,Zhi-Wen Yang,Xiangyang Yao,Xiao-Yang Li,Liang-Nian He
Graphical CO 2 photoreduction : Toward building robust artificial photosynthetic systems, a series of single-active-site rhenium bipyridyl complexes with dipyrromethene-BF 2 units exhibit outstanding catalytic efficiency for visible light-driven-CO 2 reduction. New rhenium bipyridyl complexes with dipyrromethene-BF 2 chromophores (A-ReBDP-CZ, A-ReBDP 2 , ReBDP-CZ, and ReBDP 2 ) were developed for highly efficient photocatalytic carbon dioxide (CO 2 ) reduction to carbon monoxide (CO). These catalysts consisted of two moderate electron-deficient groups (dipyrromethene-BF 2 , BDP) as the visible-light-harvesting antenna as well as both electron donor ( N -phenylcarbazole, CZ) and acceptor (BDP) on Re bipyridyl framework. Among ReBDP-CZ and ReBDP 2 complexes, the ReBDP 2 incorporating two electron-deficient BDP chromophores had a longer-lived photoexcited state (182.4 μs) and a twofold enhanced molar absorption coefficient ( ϵ =157000 m −1 cm −1 ) compared with ReBDP-CZ. Thus, ReBDP 2 achieved the superior photocatalytic reactivity and stability with a CO turnover number (TON CO ) value as high as 1323 and quantum yield ( Φ CO ) up to 55 %, which was the most excellent photocatalysis efficiency among the single-active-site Re catalysts without additional photosensitizer. Furthermore, the acetylene-bridged linker was detrimental to the photoactivity and durability of the catalyst. In brief, two BDP-based Re bipyridyl systems with outstanding catalytic performance and significant visible-light-harvesting capabilities in the solar spectrum offer a promising strategy for solar-to-fuel conversion schemes.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Jinyin Lv,Xuerong Zhou,Jianhua Yang,Lei Wang,Jinming Lu,Gaohong He,Yingchao Dong
A well-intergrown and defect-free tubular KAUST-7 membrane was fabricated via in-situ synthesis assisted by fluorinated molecular building block using green solvent of water on coarse asymmetric α-Al 2 O 3 tubes. The strategy averted the serious corrosion of high-concentration hydrofluoric acid (HF) to α-Al 2 O 3 supports due to the substitution of HF with the pre-synthesized NiNbOF 5 , overcoming the difficulty of serious corrosion to supports compared to traditional one-pot synthesis. The pH manipulation of synthesis solution is proved crucial to the fabrication of defect-free KAUST-7 membranes. In addition, effects of reactant concentration, crystallization temperature and reaction solvents on the morphology and separation performance of KAUST-7 membrane were investigated. The optimized KAUST-7 membrane M4 exhibited a H 2 perm-selectivity of 17.7 over CO 2 for H 2 /CO 2 binary mixture with a H 2 permeance of 2.2 × 10 −7 mol m −2 s −1 Pa −1 at 25 °C and 1 bar, while the H 2 /CO 2 separation factor just had a slight decrease when test temperature increased to 120 °C. The formation mechanism of KAUST-7 membranes via in-situ method in this work was investigated by exposing a bare α-Al 2 O 3 tube into NiNbOF 5 aqueous solution at the pH of 4.0 at 130 °C for 12 h. XPS and FT-IR observations revealed the formation of AlF x O y or AlF x species, which were deduced to be acted as linkers to connect with 2D Ni (II)-pyrazine layers, promoting the heterogeneous nucleation of KAUST-7 crystals on the surface of Al 2 O 3 support.
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POLYMER
·
2022
·
IF 4.432
Hongzhou Xie,Hongxu Meng,Linbo Wu,Bo-Geng Li,Philippe Dubois
Poly(ethylene 2,5-furandicarboxylate) (PEF) is a promising biobased polymer possessing high strength , rigidity and gas barrier performance, but its poor ductility and toughness may limit its practical applications. In order to obtain PEF materials with improved ductility and impact toughness as well as high strength, modulus and excellent gas barrier performance, PEF with relatively low molecular weight was modified with aliphatic polycarbonate (APC) diols by chain extension/coupling in this study. The resulting products were mixtures composed of randomly segmented copolymers , chain extended APC and chain extended PEF. The APC moiety was proved to be partially miscible with the PEF matrix, and therefore plasticized the PEF matrix and promoted its cold crystallization. In comparison with PEF, the modified PEFs possess significantly enhanced tensile ductility and impact toughness. Particularly, the modified PEF containing 15 wt% poly(hexamethylene carbonate) exhibits balanced mechanical properties and CO 2 barrier 5 times to PET .
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2022
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IF 0.847
Wei-Feng YOU,Xiao XU,Ai-Hui CAO,Zhi-Jie TAO,Long-Tian KANG
The electrocatalysts containing cobalt-pyrrolic nitrogen-carbon (Co-N 4 -C) moiety for CO 2 reduction reaction (CO 2 RR) have caught much attention. However, the effects of Co valence state and its synergy with graphene substrate are not clear yet. In this work, cobalt porphyrin (CoTPP) molecule with the intrinsic Co-N 4 -C moiety is successfully combined with graphene oxide (GO) via three kinds of liquid-phase methods. The ratio of CoTPP to GO and the valence state of Co atom are studied to explore their catalysis for CO 2 RR to CO. It is found that axially-coordinated Co(III)TPPCl/GO nanocomposites synthesized via a chemical method exhibit better ability for CO 2 RR, as compared with Co(II)TPP+GO and/or Co(III)TPPCl+GO nanocomposites obtained via a physically mixing way. After optimizing the ratio of CoTPP to GO, the Faradaic efficiency (FE) is more than 90% for CO 2 RR to CO between –0.7 and –0.8 V vs . reversible hydrogen electrode (RHE) in Co(III)TPPCl/GO75. The synergy between CoTPP and GO and the effect of Co valence state are systematically investigated, indicating that their strong interaction plays the key role in electrocatalytic CO 2 RR.
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