ACS Applied Energy Materials
·
2021
·
IF 6.024
Yuyao Zhang,Wen Chen,Min Zhou,Guobin Miao,Yueli Liu
Photoreduction of CO2 into useable hydrocarbon fuels has been widely used in the energy conversion field. However, the high carrier recombination rate and the low conversion efficiency of as-prepared catalysts greatly restrict their photocatalytic application. Herein, we synthesize Ti3C2/CsPbBr3 quantum dot (Ti3C2/CsPbBr3 QD) composites by the method of self-assembly, which are used in the photoreduction of CO2. As a result, Ti3C2/CsPbBr3 QD composites exhibit excellent photocatalytic activity and stability for the photocatalytic CO2 reduction. Especially, the generation rate of CO (17.98 μmol h–1 g–1) for Ti3C2/CsPbBr3 QD composites is 9.37 times higher than that of CsPbBr3 QDs (1.92 μmol h–1 g–1), and 97.35% of the activity is still retained after three consecutive cycles. The improved photocatalytic performance is mainly attributed to the construction of the type II-2 heterojunction as the built internal electric field (IEF) in the p–n junction could accelerate the separation for both photoinduced holes and electrons. Therefore, this work provides an insight into the construction of heterojunction photocatalysts with halide perovskite QD materials for photocatalytic applications.
研究领域:
材料科学
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能源化学
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环境科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Weiyang Yuan,Shuzhen Chen,Changlei Qin,Dawid Piotr Hanak,Xu Zhou
CO2 adsorption is an important approach to control the excessive CO2 emission from energy and industrial plants and mitigating the greenhouse effect. As an acknowledged high-temperature adsorbent, Li4SiO4 shows advantages in capturing a large amount of CO2 with a fast reaction rate and excellent cyclic stability. However, its CO2 adsorption capacity would be significantly affected by the flue gas impurities, such as SO2 and O2. The underlying reaction mechanism of such impurities and Li4SiO4 is still unclear. For this reason, this work studied the reaction path and kinetics between Li4SiO4 and SO2 through experiments, thermodynamic calculations, and characterizations. The results showed that Li4SiO4 reacts with SO2 to produce Li2SiO3 and Li2SO4 in the presence of O2 at 500–700 °C and forms Li2SiO3 and Li2SO3 in the absence of O2 at 500–682 °C. Furthermore, this study revealed a very low activation energy of 7.47 kJ/mol for Li4SiO4 sulfation in the presence of O2 in the kinetic-controlled stage, and the value goes up to 249.7 kJ/mol in the diffusion-controlled stage. These results will provide valuable references for the industrial applications of CO2 adsorption by Li4SiO4.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Shanshan Wu,Meng Tian,Yang Hu,Nan Zhang,Wei Shen,Jianyi Li,Linchuan Guo,Pengfei Da,Pinxian Xi,Chun-Hua Yan
Formate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO2 modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Debo He,Wenji Ruan,Jibiao Li,Jiupai Ni,Chengsheng Ni
The large-scale integration of intermittent renewable energies into the power grid could reduce the CO 2 emission from the combustion of fossil fuel, but it requires energy storage techniques to balance the energy production and demand. The electrolysis of CO 2 that converting electricity into chemicals/fuels provides a sustainable way of energy storage and CO 2 reduction. Solid oxide electrolysis cell (SOEC) operating at around 800 °C was able to provide highly efficient transformation of CO 2 because the high temperature was able to decrease the energy demand and increase the activation of CO 2 than room temperature electrolysis. In this study, Mo-doped ferrite perovskite , La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 , was studied as the cathode of an SOEC for the direct electrolysis of CO 2 at 800 °C. Cell with La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode showed a significantly higher current density during CO 2 electrolysis than the one with La 0.55 Sr 0.45 FeO 3 cathode. Compared with the parent La 0.55 Sr 0.45 FeO 3 cathode that will subject to a superficial decomposition into Fe 0 and SrO or SrCO 3 at an elongated cathodic bias of − 1.4 V, Mo-doping will induce the production of Ruddlesden-Popper phase ( e.g. (La,Sr) 2 (Mo,Fe)O 4 , Fe-Mo-O oxides and Fe 0 ). La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode was found to an unobvious current decrease at − 1.1 V, but a cell degradation was found under a high bias of − 1.4 V. During the 97 h’ aging under a cathodic bias (−1.4 V), the reduced molybdenum cation in La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 was found to be less mobile than Fe 3+/2+ , La 3+ or Sr 2+ , and the perovskite with Fe-deficit region were also found to be important for the activation of CO 2 and dissociation of CO in the electrochemical process.
研究领域:
材料科学
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电化学
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能源存储
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 24
·13696-13704
·
IF 3.049
Hong Lei,Ruheng Zheng,Yeping Liu,Jiacheng Gao,Xiang Chen,Xiaoliang Feng
Hydrogenation of CO2 to chemicals is of great importance in the reduction of greenhouse gas emission. And the interaction and/or the boundary between Cu and ZnO played a crucial role in the performance of the Cu–ZnO catalyst for CO2 hydrogenation to methanol. In this work, cylindrical shaped ZnO was first synthesized via controlled hydrothermal precipitation of Zn(CO2CH3)2·2H2O, and Cu was further deposited on ZnO via in situ reduction in aqueous solution. Characterizations indicated that the crystallization degree of ZnO decreased with the increasing content of Cu, while the exposed surface area of Cu exhibited a volcano shaped curve. It was found that the cylindrical shaped ZnO combined Cu catalysts were active for the hydrogenation of CO2, and the space time yield of methanol reached 0.50 g-MeOH (g-cat h)−1 at H2/CO2 = 3, 240 °C, 3.0 MPa, and 0.54 mol (g-cat h)−1, but the methanol selectivity decreases with the reduction of the (002) polar plane of ZnO. The conversion of CO2 and methanol selectivity were discussed with the detected exposed Cu surface area and the number of oxygen vacancies.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Baofei Sun,Wei Chen,Yanyi Huang,Daofu Wu,Heng Luo,Faguang Kuang,Hongmei Ran,Yichen Liu,Liqin Gao,Jinchen Zhou,Bo Gao,Qiang Huang,Xiaosheng Tang
Metal halide perovskites (MHP) are potential candidates for the photocatalytic reduction of CO 2 due to their long photogenerated carrier lifetime and charge diffusion length. However, the conventional long-chain ligand impedes the adsorption and activation of CO 2 molecules in practical applications. Here, a ligand modulation technology is employed to enhance the photocatalytic CO 2 reduction activity of lead-free Cs 2 AgInCl 6 microcrystals (MCs). The Cs 2 AgInCl 6 MCs passivated by Oleic acid (OLA) and Octanoic acid (OCA) are used for photocatalytic CO 2 reduction. The results show that the surface defects and electronic properties of Cs 2 AgInCl 6 MCs can be adjusted through ligand modulation. Compared with the OLA-Cs 2 AgInCl 6 , the OCA-Cs 2 AgInCl 6 catalyst demonstrated a significant improvement in the catalytic yield of CO and CH 4 . The CO and CH 4 catalytic yields of OCA-Cs 2 AgInCl 6 reached 171.88 and 34.15 µmol g −1 h −1 which were 2.03 and 12.98 times higher than those of OLA- Cs 2 AgInCl 6 , and the total electron consumption rate of OCA-Cs 2 AgInCl 6 was 615.2 µmol g −1 h −1 which was 3.25 times higher than that of OLA-Cs 2 AgInCl 6 . Furthermore, in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs 2 AgInCl 6 MCs induced by ligand modulation. This study illustrates the potential of lead-free Cs 2 AgInCl 6 MCs for efficient photocatalytic CO 2 reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Menglei Mao,Feixue Sun,Ruqing Chong,Rui Gao,Qiyong Liao,Zihui Meng,Xinlong Fan,Wenfang Liu
Ti 3 C 2 T x as a typical MXene material has a multilayer structure similar to accordion, whose interlayer spacing and specific surface area can be regulated by intercalation and modification. In this work, the effects of several kinds of cation-containing intercalators including NH 4 OH, KOH and NH 4 OH/KCl on the structure of Ti 3 C 2 T x and its application performance in enzymatic CO 2 conversion were investigated for the first time. The results show that Ti 3 C 2 T x intercalated with NH 4 OH/KCl had larger layer spacing (25.25 Å) and specific surface area (20.85 m 2 /g), and better enhancing effect. The initial reaction rate was 0.379 mM/h, which was separately 1.04, 1.42, 1.76 and 5.29 times that of Ti 3 C 2 T x /KOH, Ti 3 C 2 T x /NH 4 OH, Ti 3 C 2 T x and the blank system. Following that, Ti 3 C 2 T x /NH 4 OH/KCl was modified by polyethyleneimine (PEI) and dopamine (DA) and the concentration of modifier was optimized. PEI modified Ti 3 C 2 T x /NH 4 OH/KCl (PEI-Ti 3 C 2 T x ) was superior to PEI/DA modified that in the N content, CO 2 adsorption capacity and application performance. With the addition of 20 mg PEI-Ti 3 C 2 T x , the initial reaction rate was 0.658 mM/h, which was 1.74 and 9.2 times that of before modification and the blank system, respectively. PEI-Ti 3 C 2 T x also exhibited a good reusability and the initial reaction rate was 89.4% of the initial value after 10 cycles.
研究领域:
材料科学
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环境科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Dan Li,Cuiping Li
A class of CO2-binding organic liquids (CO2-BOLs) composed of 1,1,3,3-Tetramethylguanidine (TMG) and Glycerol (Gly) and Gly’s amino derivatives were developed for highly efficient and reversible CO2 capture. These CO2-BOLs exhibited high gravimetric CO2 solubility up to 0.196 g CO2·g–1 at 313.2 K and 1.0 atm, superior to most functionalized ILs and other absorbents. The influential factors of CO2 absorption, such as components of CO2-BOLs, absorption temperature, and CO2 partial pressure together with water contents were investigated, and the recyclability of CO2-BOLs was verified to be excellent. The absorption mechanism of CO2-BOLs was explored with the help of spectral analysis, quantum chemical calculation, and thermodynamic analysis. All the results revealed that chemisorption took place once these CO2-BOLs were exposed to CO2, and alkyl guanidine carbonates were produced. Besides, it is illustrated that introducing the amino group to Gly could reduce the nucleophilic reactivity of CO2-BOLs, along with the absorption enthalpy simultaneously.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Wenji Zheng,Jingbang Yu,Zhongyue Hu,Xuehua Ruan,Xiangcun Li,Yan Dai,Gaohong He
Layered double hydroxide (LDH) bearing numerous hydroxyl groups shows high affinity with CO 2 and is promising in mixed matrix membranes (MMMs) based CO 2 capture. However, its non-porous structure limits the further improvement of CO 2 permeability. In this work, 3D hollow CoNi-LDH nanocages were developed to construct low-resistance and CO 2 -philic transport channel in MMM by in-situ etching of ZIF-67 template. The resultant material exhibits hollow structure with cavity size of about 500 nm, mesopores and micropores from LDH stacking and ZIF-67 template. The outer layered CoNi-LDH nanosheets can attract more CO 2 molecules by their abundant hydroxyl groups, resulting in an improvement in dissolution selectivity of CO 2 over N 2 . Meanwhile, the tortuous gas diffusion paths originated from 2D nanosheet stacking can further enhance the CO 2 selectivity over N 2 . Moreover, the hollow nanocages provide CO 2 molecules with fast transport path, resulting in high CO 2 permeability. As a result, compared with pure Pebax membrane and 2D LDH/Pebax MMM, all the 3D hollow CoNi-LDH/Pebax MMMs present enhanced CO 2 permeability. The 3D hollow CoNi-LDH-2h/Pebax MMM performs the highest CO 2 permeability of 135.49 Barrer, which are increased by 141.95% and 71.50% than those of the above two membranes, respectively. The selectivity of 3D hollow CoNi-LDH-2h/Pebax MMM is about 26.30% higher than that of the pure Pebax membrane. The present membrane presents comparable CO 2 capture capacity in contrast with most reported Pebax based MMMs and surpasses the Robeson upper bond. Together with the good long-term stability, the 3D hollow CoNi-LDH nanocages are believed to be a promising candidate for MMMs to improve CO 2 capture.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Chem Catalysis
·
2023
·
IF 9.4
Rong Wang,Yue Peng,Jane Chung,Zhen Chen,Xiyang Wang,Haibo Yin,Yimin A. Wu,Jingshan Luo,Junhua Li
Summary The electrocatalytic reduction of CO 2 is an attractive method for reducing greenhouse gases and producing chemical feedstocks. However, the activation of C=O bonds limits the reaction kinetics; therefore, understanding the mechanism of C=O bond activation can guide the design of high-performance catalysts. Here, we investigate the C=O bond activation mechanism during the electroreduction of CO 2 to CO on ZnO. Using in situ experimental techniques and quantum chemical calculations , we find that defects in ZnO promote the formation of Zn–ZnO x interfaces during CO 2 reduction, which mediates an intimate-junction exciton state by the metal semiconductor heterophase. This promotes the formation of CO 2 radicals, exposing electron donation centers for CO 2 adsorption and redox centers for cleaving stable C=O bonds. The internal electric field generated by the heterojunction enhances the initial C=O activation by facilitating the interaction between the metalized Zn d-orbital and the O π -orbital in CO 2 .
研究领域:
电化学
·
材料科学
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催化
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Da Wang,Ying Zhu,Weiting Yu,Zhiqiao He,Feilong Dong,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Lizhang Wang,Shuang Song
Ag-based electrodes have emerged as important candidates for the industrial electrochemical CO 2 reduction reaction (eCO 2 RR) to form CO. Herein, an intrinsic versatile Ag electrode has been derived in situ from Ag-MOF on Ag foam (denoted as ER-AF), which exhibits the highest current density (57.2 mA cm −2 ) at a potential of −1.15 V vs. RHE reported to date for the formation of CO in a commonly used H-type cell. ER-AF has multiple-roles: The 3D dendrite structure promotes mass diffusion; the rich edges sites favor CO 2 adsorption and conversion, and the highly exposed (111) facet facilitates the desorption of CO. Their cooperating functions result in the remarkable performance of ER-AF in the eCO 2 RR to form CO. This work offers an effective strategy to achieve high eCO 2 RR activity and selectivity by assembling the active and stable sites together on the MOF-derived materials.
研究领域:
电化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2016
·Vol. 6
·期 1
·1-10
·
IF 5.228
Feng Anchao,Liang Jiamei,Ji Jinzhao,Dou Jinbo,Wang Shanfeng,Yuan Jinying
Despite numerous studies on utilizing polymeric vesicles as nanocapsules, fabrication of tunable molecular pathways on transportable vesicle walls remains challenging. Traditional methods for building penetrated channels on vesicular membrane surface often involve regulating the solvent polarity or photo-cross-linking. Herein, we developed a neat, green approach of stimulation by using CO 2 gas as “molecular drill” to pierce macroporous structures on the membrane of polymersomes. By simply introducing CO 2 /N 2 gases into the aqueous solution of self-assemblies without accumulating any byproducts, we observed two processes of polymeric shape transformation: “gas breathing” and “gas piercing.” Moreover, the pathways in terms of dimension and time were found to be adjustable simply by controlling the CO 2 stimulation level for different functional encapsulated molecules in accumulation, transport, and releasing. CO 2 -breathing and piercing of polymersomes offers a promising functionality to tune nanocapsules for encapsulating and releasing fluorescent dyes and bioactive molecules in living systems and also a unique platform to mimic the structural formation of nucleus pore complex and the breathing process in human beings and animals.
研究领域:
生物化学
·
纳米医学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）