ACS Catalysis
·
2021
·
IF 13.084
Huiyuan Cheng,Xuemei Wu,Manman Feng,Xiangcun Li,Guangping Lei,Zihao Fan,Dongwei Pan,Fujun Cui,Gaohong He
Developing diatomic catalysts (DACs) for the CO2 reduction reaction (CO2RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, the proper design of DACs at an atomic level and an understanding of the synergistic mechanism of binary sites remain challenging. Herein, an N-rich carbon matrix with precisely controlled Ni/Cu dual sites is synthesized through the assistance of metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency of over 95% from −0.39 to −1.09 V vs reversible hydrogen electrode (RHE) with the maximum value of 99.2% at −0.79 V vs RHE and long-term durability of 60 h electrolysis. Density functional theory studies reveal that the electronic redistribution and band gap narrowing induced by the adjacent NiN4 and CuN4 moieties enhance the electron conductivity and strengthen the bonding interactions between *COOH intermediates and Ni centers, thus lowering the overall reaction barriers and promoting CO generation.
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高影响因子
LANGMUIR
·
2020
·
IF 3.557
Yangguan Chen,Guorong Lin,Shuixia Chen
Amine-skeleton solid-amine materials are promising adsorbents for CO2 capture from flue gas. Here, a novel solid-amine microsphere was synthesized by cross-linking the skeleton poly(ethylenimine) (PEI) with ethylene glycol diglycidyl ether in a facile one-pot W/O emulsion system. The material had a remarkable CO2 adsorption capacity of 7.28 mmol/g in the presence of moisture at 20 °C, 0.1 bar. The highest ratio of breakthrough capacity to saturation capacity was ca. 84%. According to kinetic simulation, the Avrami kinetic model could better describe the adsorption process of CO2 under different temperatures, in which the value of R2 was above 0.99 and n was between 1 and 2, indicating that both physical and chemical adsorption mechanisms were performed during adsorption. Moreover, the material had a high swelling speed. Equilibrium was established within 30 s, and the swelling ratio was 271% at equilibrium. The saturated adsorbent could be easily regenerated with a regeneration efficiency of 94.63% after six cycles. The PEI microsphere appears to be a promising candidate material for CO2 capture from flue gas.
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高影响因子
ACS Applied Bio Materials
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2020
·
IF 0
Xinke Kong,Panpan Gai,Feng Li
Biohybrid photoelectrochemical systems could combine the light-harvesting ability of semiconductor photocatalysts and the CO2-processing capability of biocatalysts to realize CO2 reduction. How to develop the energy-utilized model can be of importance for the mechanism exploration of photosynthesis. Here, a biohybrid photoelectrochemical system based on HCOO––CO2 circulation was developed to realize the conversion both of solar-to-electric energy and chemical-to-electric energy. The device consists of a TiO2 nanoparticle photoanode and a laser-scribed graphene/formate dehydrogenase biocathode, which was utilized for the formic acid oxidation and the biocatalysis reduction of CO2 to HCOO–, respectively. The as-proposed biohybrid photoelectrochemical system exhibits good performance with an open-circuit potential of 0.93 V and a maximum power output density of 76 μW cm–2. This ingenious strategy not only exploits a robust carbon circulation system for the conversion of solar energy but also provides a way of constructing complex artificial photosynthesis systems.
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Journal of Cleaner Production
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2022
·
IF 11.072
Shunan Yin,Jinxian Zhao,Shiping Wu,Xuhui Wang,Yanhong Quan,Jun Ren
Electrochemical reduction of CO 2 to valuable chemicals using electricity from renewable sources is a promising approach to realize the carbon cycle. Here, a novel bimetallic nitrogen-doped carbon catalyst (M-N-C, where M denotes the metal) CoCu–N–C electrocatalyst has been synthesized by pyrolyzing a copper-doped cobalt(II) acetate–phenanthroline complex formed from the metal acetates and 1,10-phenanthroline dissolved in ethanol. The optimal CoCu–N–C catalyst with molar ratio of Cu/(Co + Cu) = 0.15 displayed superior performance, enabling a faradaic efficiency of CO production of 76.5% at an overpotential of 0.57 V as well as an increased CO current density of 8.48 mA cm −2 at −0.98 V versus reversible hydrogen electrode (far superior than the Co–N–C of 4.20 mA cm −2 and Cu–N–C of 0.07 mA cm −2 ) and a decreased charge-transfer resistance compared with Co–N–C and Cu–N–C catalysts. The addition of Cu, which serves as a structure promoter to improve the dispersion of Co, thereby providing sufficient Co-N x active sites for the electrochemical CO 2 reduction reaction (CRR). Moreover, doping Cu changes the electronic environment around Co slightly and promotes the charge transfer capability so that reduces the energy barrier of potential-limiting energy, thereby improving the CRR performance of catalyst.
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高影响因子
APPLIED ENERGY
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2018
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IF 7.9
Yao Shen,Chenkai Jiang,Shihan Zhang,Jun Chen,Lidong Wang,Jianmeng Chen
The main issue related to the deployment of the absorption based technology for CO 2 capture is the intensive energy penalty. Biphasic solvent is regarded as a promising candidate for CO 2 capture due to its potential in significant reduction of the energy consumption. However, currently, the development of biphasic solvents relies on the intensity of solvent screening work. To address this issue, this work investigated the relationships between the solvent properties and CO 2 capture performance such as absorption capacity, phase separation behavior, kinetics, and thermodynamics. Ten primary/secondary amines and eight tertiary amines with different alkalinity ( pKa ) and hydrophobicity (Log P) were used as the main components of the biphasic solvent . Experimental results revealed that the tertiary amine’s alkalinity determines the absorption capacity of the biphasic solvent. The maximum CO 2 absorption capacity was achieved by the tested biphasic solvent with a tertiary amine of a pKa around 9.8. Compared with the tertiary amine, the primary amine’s hydrophobicity was more sensible to the phase separation behavior of the solvent. The low Log P value of the primary amine and the high Log P value of the tertiary amine befitted the phase separation. Kinetic analysis indicate that the total mass transfer resistance of the rich solution decreased with the increase in the Log P value of the tertiary amine. Interestingly, the highest enhancement factor was achieved by the tertiary amine (2-(diethylamino)ethanol) with the pKa of 9.79. Further increase of the tertiary amine’s pKa decreased the enhancement factor of the biphasic solvent. This was attributed to the limitation of mass transfer of tertiary amine from the upper phase to lower phase. Furthermore, thermodynamic analysis showed that the sensible heat and the latent heat of the solvents decreased and increased, respectively, with the increase of log P value of the tertiary amines. The lowest reaction enthalpy and heat duty of the tested biphasic solvents were 45.8% and 52% lower than those of the benchmark monoethanolamine solution, respectively. Overall, compared with the primary amine, the selection of the tertiary amine is more important to achieve a great performance for CO 2 capture. Therefore, the tertiary amine with a moderate pKa and Log P is beneficial to achieve a high absorption capacity, fast absorption rate, and low heat duty of the biphasic solvent.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bowen Lu,Ziqiang Han,Xinyu Zhi,Liqi Zhang
NiFe 2 O 4 exhibits excellent redox properties and is widely applied in catalytic reactions. However, rapid inactivation under reaction conditions limited its industrial applications. In this study, CeO 2 -NiFe 2 O 4 composite catalysts were synthesized, and the Reverse Water Gas Shift (RWGS) reaction was measured to reveal its CO 2 hydrogenation performance under a high-temperature condition. NiFe 2 O 4 catalysts got deactivated after being reduced to Fe-Ni alloy at 700 °C, decreasing the CO 2 conversion rate. CeO 2 addition can significantly improve its high-temperature activity, and 20CeO 2 -NiFe 2 O 4 exhibited the best catalytic activity (80.85 %, 700 °C). The CeO 2 -confined maintained Ni-Fe alloy with a relatively small crystal size and larger specific surface area, supporting more active sites for CO 2 hydrogenation. CeO 2 addition induced higher oxygen vacancy concentration, enhancing CO 2 activation and formates species formed on 20CeO 2 -NiFe 2 O 4 , resulting in higher CO 2 conversion activity. In addition, 20CeO 2 -NiFe 2 O 4 maintained its catalytic stability for 50 h at 700 °C. The CeO 2 confined enhanced the high-temperature stability of Fe-Ni alloy. CeO 2 and formed CeFeO 3 dispersed in 20CeO 2 -NiFe 2 O 4 inhibited excessive aggregation of Fe-Ni alloy, and CeO 2 inhibited carbon deposition on Fe-Ni alloy, improving Fe-Ni alloy’s reaction stability under RWGS reaction conditions. CeO 2 confined may give insight into improving metal stability under high-temperature and reductive conditions in heterogeneous catalysis.
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高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-9
·
IF 14.919
Liang Chu,Chen Yun,Wu Min,Wang Kai,Zhang Wenkui,Gan Yongping,Huang Hui,Chen Jian,Xia Yang,Zhang Jun,Zheng Shiyou,Pan Hongge
Environmentally benign synthesis of graphite at low temperatures is a great challenge in the absence of transition metal catalysts. Herein, we report a green and efficient approach of synthesizing graphite from carbon dioxide at ultralow temperatures in the absence of transition metal catalysts. Carbon dioxide is converted into graphite submicroflakes in the seconds timescale via reacting with lithium aluminum hydride as the mixture of carbon dioxide and lithium aluminum hydride is heated to as low as 126 °C. Gas pressure-dependent kinetic barriers for synthesizing graphite is demonstrated to be the major reason for our synthesis of graphite without the graphitization process of amorphous carbon. When serving as lithium storage materials, graphite submicroflakes exhibit excellent rate capability and cycling performance with a reversible capacity of ~320 mAh g –1 after 1500 cycles at 1.0 A g –1 . This study provides an avenue to synthesize graphite from greenhouse gases at low temperatures.
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高影响因子
RARE METALS
·
2024
·Vol. 43
·期 4
·1513-1523
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IF 9.6
Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen
Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract
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高影响因子
Nano Energy
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2019
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IF 15.548
Changfan Xu,Kaiwen Zhang,Da Zhang,Shilei Chang,Feng Liang,Pengfei Yan,Yaochun Yao,Tao Qu,Jing Zhan,Wenhui Ma,Bing Yang,Yongnian Dai,Xueliang Sun
A reversible long-life hybrid Na-CO 2 battery is proposed by using Na 3 Zr 2 Si 2 PO 12 solid electrolyte as a separator, N-doped single-wall carbon nanohorns (N-SWCNH) as a catalyst and the saturated NaCl solution as an aqueous catholyte. The Na 3 Zr 2 Si 2 PO 12 ceramic not only has high Na + ion conductivity, but also prevents potential contamination from H 2 O and CO 2 to sodium anode, and avoids the internal short-circuit touch of Na dendrite with cathode, improving the safety of the battery. Benefiting from N dopants , unique internal and interstitial nanoporous structures, N-SWCNH have large surface area for discharge products accumulation, offer substantial structural defect sites for CO 2 adsorption and electron transfer , contributing to high catalytic activity and reversibility . Most importantly, the hybrid Na-CO 2 battery with aqueous electrolyte facilitates the dissolution of the insulated discharge product, which overwhelmingly improves the discharge and charge reactions kinetics. Na-CO 2 batteries exhibit a low charging voltage of 2.62 V and a small voltage gap of 0.49 V at a current density of 0.1 mA cm −2 , a superior discharge capacity of 2293 mAh·g −1 at a current density of 0.2 mA cm −2 , a high round trip efficiency of ~68.7% after 300 cycles. In-situ Raman and ex-suit XRD analyses convincingly show that NaHCO 3 and carbon are the main discharge products.
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高影响因子
LANGMUIR
·
2014
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IF 4.384
Pingwei Liu,Weiqiang Lu,Wen-Jun Wang,Bo-Geng Li,Shiping Zhu
Cross-linked polymer particles were prepared via surfactant-free emulsion copolymerization of 2-(diethylamino)ethyl methacrylate (DEAEMA) and sodium methacrylate (SMA) using N,N′-methylenebis(acrylamide) (MBA) as a cross-linker. Generated particles are zwitterionic, possessing unique isoelectric points in the pH range of 7.5–8.0, which is readily tunable through CO2/N2 bubbling. The particles were found to be highly responsive to CO2/N2 switching, dissolving in water with CO2 bubbling and precipitating with N2 bubbling at room temperature. Pickering emulsions of n-dodecane were prepared using these particles as the sole emulsifier. These emulsions can be rapidly demulsified with CO2 bubbling, resulting in complete oil/water phase separations. Nitrogen bubbling efficiently re-emulsifies the oil with the aid of homogenization. The rapid emulsification/demulsification using CO2/N2 bubbling at room temperature provides these cross-linked zwitterionic particles with distinct advantages as functional Pickering surfactants.
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高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2024
·Vol. 40
·期 3
·484-489
·
IF 3.1
Xiao Qi,Liu Ting,Zhou Qianhe,Li Liangyu,Chang Chuntao,Gao Dawei,Li Danyang,You Feifei
Photocatalytic CO 2 reduction driven by solar light is a green approach that can decrease the greenhouse effect induced by high CO 2 concentration in the atmosphere and generate carbon-based chemicals/fuels as well. In this paper, non-metal co-catalysts ZnO/ZnS type-II hetero-junction nanoparticles with a rough surface were prepared through a hydrothermal process. When used as a photocatalyst for CO 2 reduction, the optimal one showed good cycle stability and a higher yield rate of 27.8 µmol·g −1 ·h −1 for CO 2 conversion into CO. The outstanding catalytic activity originated from i) the rich interfaces between ZnO and ZnS in the nanoscale could significantly reduce the delivery path of carriers and improve the utilization efficiency of photo-excited electron/hole pairs and ii) enriched surface oxygen defects could supply much more reaction active sites for CO 2 adsorption.
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高影响因子
Nanoscale Research Letters
·
2018
·Vol. 13
·期 1
·1-7
·
IF 3.125
Tang Nian,He Tingyu,Liu Jie,Li Li,Shi Han,Cen Wanglai,Ye Zhixiang
The interlamellar spacing of layered double hydroxides (LDHs) was enlarged by dodecyl sulfonate ions firstly, and then, (3-aminopropyl)triethoxysilane (APS) was chemically grafted (APS/LDHs). The structural characteristics and thermal stability of these prepared samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), reflectance Fourier transform infrared spectrometer (FTIR), thermogravimetric analysis (TG), and elemental analysis (EA) respectively. The CO 2 adsorption performance was investigated adopting TG and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The results presented that the CO 2 adsorption capacity on APS/LDHs was as high as 90 mg/g and showed no obvious reduction during a five cyclic adsorption-desorption test, indicating its superior performance stability. The DRIFTS results showed that both carbamates and weakly bounded CO 2 species were generated on APS/LDHs. The weakly adsorbed species was due to the different local chemical environment for CO 2 capture provided by the surface moieties of LDHs like free silanol and hydrogen bonds.
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高影响因子
危险品化学品经营许可证（带存储）