APPLIED ENERGY
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2022
·
IF 11.446
Boshu Jiang,Bachirou Guene Lougou,Hao Zhang,Boxi Geng,Lianxuan Wu,Yong Shuai
The solar-driven thermochemical CO 2 -to-CO conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality. However, synthesizing porous reacting materials with excellent thermal stability, hardness and long-term cyclic stability, oxygen exchange capacity, and higher CO 2 -to-CO conversion are the most important challenges associated with the thermochemical CO 2 -splitting approach and technological upscaling to large-scale applications. This study presented the development of NiFe 2 O 4 oxygen carriers, the synthesis method of SiC and Si 3 N 4 supports, and solar-to-fuel processing of the newly prepared materials through CO 2 -splitting under a highly concentrated solar radiative heat flux. The newly synthesized NiFe 2 O 4 @SiC porous redox material resulted in higher solar energy absorption and CO 2 conversion capability with an instantaneous CO production of 410 μmol/g and direct CO 2 -to-CO conversion rate of 18.1 % at 1073–1273 K reaction temperature. The media composite of NiFe 2 O 4 @SiC exhibited high-temperature thermal changes, good thermochemical reaction stability, and a higher CO production rate through six redox cycles compared to NiFe 2 O 4 @Si 3 N 4 porous reacting material. The high oxidation potential and remarkably solar radiative heat flux absorption and thermochemical CO 2 -splitting capacities of the newly developed materials were demonstrated through experimental analysis. The synergistic effect of the oxygen carriers (NiFe 2 O 4 ) and substrate materials including SiC and Si 3 N 4 skeletons for CO 2 -splitting is highlighted. This study provided comprehensive and novel experimental insights that can be used as guidance for theoretical research and application in CO 2 conversion into high-value-added energy products.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yun Li,Houfang Lu,Yingying Liu,Kejing Wu,Yingming Zhu,Bin Liang
Nano-SiO 2 was used to enhance the performance of CO 2 absorption and desorption in viscous DBU-glycerol solution with a viscosity of about 60 mPa·s. The effects of ultrasonic time in the preparation of nanofluids, solids loading and particle/cluster size of SiO 2 on absorbent properties and absorption performance were investigated. Meanwhile, the enhancements of heat transfer and mass transfer with nanoparticles in the desorption of CO 2 -loaded DBU-glycerol solutions were also analyzed. Proper ultrasonic vibration time and nano-SiO 2 loading can both decrease the average particle size in the system which can improve the absorption. The increase of interfacial area between gas and liquid with the addition of nano-SiO 2 dominates the enhancement of absorption and it has little effect on the enhancement factor when the nano-SiO 2 size is 102 nm or below. But when the particle size is higher than 102 nm, the enhancement factor decreases with the increase of particle/cluster size. The addition of 0.10 wt% SiO 2 nanoparticle with a particle size of 16 nm can increase the absorption rate by 31 % compared with base liquid. In desorption process, the desorption rate for CO 2 -loaded DBU-glycerol solutions can increase 18 % with the addition of 0.10 wt% nano-SiO 2 with a particle size of 32 nm. The main reason could be that nano-SiO 2 can improve the heating rate of the base fluid and supply plenty of nucleation sites for the formation of bubbles to improve the desorption rate. It shows that nano-SiO 2 can be used to enhance both the absorption and desorption processes in solutions with high viscosity.
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JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 30
·期 3
·889-897
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IF 2.523
Hu Lihua,Chen Li,Mo Xiaohong,Peng Xiong,Xu Wei,Liu Feng,Yan Zongcheng
For the effective utilization of carbon resources, a facile and recyclable heterogeneous catalyst system with high reactivity and stability is urgently needed for chemical fixation of CO 2 . Herein, a micro/nanostructured ZIF-8/CeO 2 composite was designed by direct surface-nucleated ZIF-8 nanoparticles on spindle-like CeO 2 . The ZIF-8 nanoparticles content of the ZIF-8/CeO 2 composite could be tuned by the changing of reaction parameters, such as the molar ratio of reactants and the reaction time. The ZIF-8/CeO 2 composite exhibits remarkably enhanced catalytic activity and superior reusability for cycloaddition reaction of CO 2 and epoxide than its pure substance. The enhanced performance of ZIF-8/CeO 2 composite should be attributed to its high specific surface area and abundant porosity, outstanding thermal stability, and the appearance of a new moderate acid/base site in composite material. Considering the convenient preparation, enhanced catalytic activity and excellent reusability of ZIF-8/CeO 2 composite, this work offers a new strategy to replace ZIFs-based porous catalysts for chemical fixation of CO 2 .
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Zhiyong Zhu,Guanyao Yu,Liangjing Duan,Xiao Liu,Li Wang,Jinglai Zhang
Developing a robust catalyst for CO 2 reduction reaction (CO 2 RR) is critical to achieving a closed carbon cycle. Yet, the process of CO 2 RR still faces enormous challenges, in part because of the lack of highly active, stable, as well as cost-effective electrocatalysts. In this work, we reported an effective and sample strategy to immobilize nickel phthalocyanine (Ni-Pc) molecules on the fruit-peel-derived carbon framework surface (denoted as Ni-Pc/CF and carbon framework denoted as CF) with exceptional CO production performances. Dispersed Ni-Pc molecules on the carbon materials are verified by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman measurements. The obtained Ni-Pc/CF catalyst shows that the high faradaic efficiency (FE) exceeds 95.0 % over a potential of −0.7 to −0.9 V ( vs reversible hydrogen electrode (RHE), V RHE ), the maximum FE (99.1 %) can close to 100 % at −0.8 V, and the excellent stability over a 10 h reaction period. This work offers valuable insights into the immobilization of stabilized, highly dispersed molecule catalysts on carbon materials surfaces for selective reduction of CO 2 to CO.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 16
·2214215
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IF 19
Xiaosong Hu,Xinyu Liu,Xin Hu,Chaoyue Zhao,Qingxin Guan,Wei Li
Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N 4 sites and low valence CuN x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N 4 and N 4 structures, which show strong Lewis basicity and has strong adsorption for *CO 2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO 2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO 2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO 2 . In the catalytic process, CuN x not only adsorbs and activates H 2 , but also cooperates with the adjacent Zn-N 4 and N 4 structures to jointly activate CO 2 molecules and further promotes the hydrogenation of CO 2 . This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
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ChemistrySelect
·
2023
·Vol. 8
·期 5
·e202204303
·
IF 2.1
Weishan Tang,Yunpeng Shen,Peng Yang,Caiyun Lin,Zhijun Ke,Xiaoping Rao
Graphical The single-walled carbon nanotubes dispersed by an extremely rigid CO 2 -responsive surfactant were used to fabricate highly conductive epoxy composites with ultra-strong mechanical properties. The emerging nanomaterials single-walled carbon nanotube (SWNTs) with large specific surface area, excellent electrical conductivity and high mechanical strength, has been used to fabricate electronic devices. However, the extremely strong π-π interactions make SWNTs easy to agglomerate, thus limiting their application. In this work, a novel method was applied to disperse SWNTs by using rigid rosin-based CO 2 responsive surfactant rosin acid dimaleimide choline (R-BMI-C). When pH 10.4, SWNTs can be uniformly and stably dispersed, and at pH 6.3, SWNTs aggregated. The dispersed SWNTs was then integrated into diglycidyl ether of bis phenol A (DGEBA) to fabricate high conductive epoxy composites. Their properties were characterized by SEM, TG, high resistivity meters, etc. . The results showed that the modified SWNTs/DGEBA composites obtained an ultra-low percolation threshold (0.025 wt.%). Compared with the original SWNTs/DGEBA composite, its tensile strength and elastic modulus were enhanced by 17 % and 96 %, respectively, when the SWNTs content was 0.5 wt.%.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2022
·
IF 3.119
Tiantian Ping,Qinghai Long,Shufeng Shen
Solubility of N2O and CO2 in pure 2-butoxyethanol (2-BE) was determined in a stirred equilibrium cell at temperatures ranging from 283.2 to 333.2 K and correlated as an exponential function of temperature. Ratios of solubility of CO2 to N2O in several reported solvents were found to be strongly dependent on the order of solvent dielectric constants. Solubility of N2O in 2-(butylamino)ethanol (BAE) and the binary blends of 2-BE and BAE was measured over the temperature range from 283.2 to 333.2 K and with BAE concentration from 6.5 to 65.4 mass%. N2O solubility data were well represented by correlation models with AARDs within 0.8%. Physical solubility of CO2 in a nonaqueous 2-BE/BAE system can be estimated using the N2O analogy method.
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ChemSusChem
·
2022
·Vol. 16
·期 5
·e202201956
·
IF 9.14
Xiu Xing,Yan Liu,Ru-De Lin,Yang Zhang,Zhong-Liu Wu,Xiao-Qi Yu,Kun Li,Na Wang
Graphical Tailor made ! An environmentally friendly and highly effective semi-artificial photosynthetic system (FDH@Rh-TCPP-UiO-66-NH 2 ) was developed for transforming CO 2 into formic acid. The incorporation of NADH-dependent formic acid dehydrogenase (FDH), photosensitive porphyrin ligands and Rh complex lead to highly selective and recyclable system. Herein, a Zr-based dual-ligand MOFs with pre-installed Rh complex was employed for NADH regeneration in situ and also used for immobilization of formic acid dehydrogenase (FDH) in order to realize a highly efficient CO 2 fixation system. Then, based on the detailed investigations into the photochemical and electrochemical properties, it is demonstrated that the introduction of the photosensitive meso-tetra(4-carboxyphenyl) porphin (TCPP) ligands increased the catalytic active sites and improved photoelectric properties. Furthermore, the electron mediator Rh complex, anchored on the zirconium-based dual-ligand MOFs, enhanced the efficiency of electron transfer efficiency and facilitated the separation of photogenerated electrons and holes. Compared with UiO-66-NH 2 , Rh-H 2 TCPP-UiO-66-NH 2 exhibits an optimized valence band structure and significantly improved photocatalytic activity for NAD + reduction, resulting the synthesis of formic acid from CO 2 increased from 150 μg mL −1 (UiO-66-NH 2 ) to 254 μg mL −1 (Rh-H 2 TCPP-UiO-66-NH 2 ). Moreover, the assembled photocatalyst-enzyme coupled system also allows facile recycling of expensive electron mediator, enzyme, and photocatalyst.
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PubMed
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Xing Gong,Quantao Liu,Huan Wang,Pei Wan,Shuaichao Chen,Jinyi Wu,Shaopeng Wu
The polyurethane (PU) modified asphalt prepared by melting method has poor thermal storage stability and the PU used is normally synthesized from non-renewable petrochemical resources. This paper aims to explore the feasibility of preparing environment-friendly PU and using it to enhance asphalt properties. Environmental-curable CO 2 -based PPC-PU and ordinary BDO-PU was prepared with poly propylene carbonate diol (PPC) and Butanediol (BDO), respectively. Fourier transform infrared spectroscopy and thermogravimetric analysis were used to examine their chemical compositions and thermal characteristics. Then, these two types of PU were used to modified asphalt and the chemical functional groups, microstructure, storage stability, viscosity, low temperature, and high temperature properties of various modified asphalts were tested. The findings revealed that the prepared PPC-PU and BDO-PU had good thermal stability and the decomposition temperature was above 200 °C. PPC-PU modified asphalt can be gradually cured at natural environment to form a crosslinking network, and the curing rate can reach 86.23% in 15 days. In addition to the low temperature performance, other properties of PPC-PU modified asphalt were gradually improved with the extension of curing time. Compared with BDO-PU modified asphalt, PPC-PU modified asphalt has superior storage stability, low temperature, and high temperature properties. It is concluded that the environmental-curable PPC-PU can improve performance of asphalt while consuming CO 2 . This research offers a fresh concept for producing of green PU modified asphalt.
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ADVANCED MATERIALS
·
2022
·Vol. 35
·期 5
·2205262
·
IF 32.086
Runyao Zhao,Yiding Wang,Guipeng Ji,Jiajun Zhong,Fengtao Zhang,Meifang Chen,Shengrui Tong,Peng Wang,Zhonghua Wu,Buxing Han,Zhimin Liu
Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers a promising strategy to lower CO 2 emission while producing value-added chemicals. A great challenge facing CO 2 RR is how to improve energy efficiency by reducing overpotentials. Herein, partially nitrided Ni nanoclusters (NiN x ) immobilized on N-doped carbon nanotubes (NCNT) for CO 2 RR are reported, which achieves the lowest onset overpotential of 16 mV for CO 2 -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN x /NCNT affords a CO generation rate of 43.0 mol g −1 h −1 at a low potential of −0.572 V (vs RHE). DFT calculations reveal that the NiN x nanoclusters favor *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO 2 RR overpotential. As NiN x /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm −2 , with total energy efficiency of 62.2%.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Yan Zhang,Chuang Chen,Qiu-Hui Zheng,Zhan-Kuo Guo,Bao-Xia Dong,Yun-Lei Teng
Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped NiII-triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni–S–CT (T = 800, 900, 1000 °C) materials with Ni3S2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i–t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni–S–CT catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni–S–C1000 exhibited the best catalytic activity (FECO of 66.6% and jCO of 1.28 mA/cm2). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni3S2 to illustrate the ECR activity origination. It is the first report on Ni3S2-based catalysts in the application of ECR.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Qiyou,Liu Kang,Hu Kangman,Cai Chao,Li Huangjingwei,Li Hongmei,Herran Matias,Lu Ying-Rui,Chan Ting-Shan,Ma Chao,Fu Junwei,Zhang Shiguo,Liang Ying,Cortés Emiliano,Liu Min
Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO 2 . However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO 2 activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties. In situ attenuated total reflection infrared spectroscopy and theoretical calculations demonstrate that this strategy increases the electron density around the metal centers and facilitates CO 2 activation. As a result, for the electroreduction of CO 2 to CO in aqueous KHCO 3 electrolyte, the cyano-modified catalyst exhibits a turnover frequency of ~22,000 per hour at −1.178 V versus the reversible hydrogen electrode (RHE) and maintains a Faradaic efficiency (FE) above 90% even with a CO 2 concentration of only 30% in an H-type cell. In a flow cell under pure CO 2 at −0.93 V versus RHE the cyano-modified catalyst enables a current density of −300 mA/cm 2 with a FE above 90%.
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