Journal of CO2 Utilization
·
2020
·
IF 5.993
Chengyi Dai,Xiao Zhao,Borui Hu,Xinbao Zhang,Qunxing Luo,Xinwen Guo,Xiaoxun Ma
Capturing and utilization of carbon dioxide (CO 2 ) not only leads to effective use of carbon resources, but also alleviates environmental pollution caused by increasing concentration of CO 2 , thus making it a hot research topic in recent years. In this study, a series of highly dispersed iron-cobalt (Fe-Co) catalysts was prepared by ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) modification, which could efficiently convert CO 2 into high value-added chemicals (C 2 -C 4 = and C 5 -C 11 ). X-ray diffraction (XRD) analysis showed that the addition of a small amount of Co and EDTA-2Na contributed to enhance the sintering resistance of Fe species. During the calcination process, EDTA 4− can be decomposed into small organic molecules with reducibility, thus promoting the reduction of iron species. The CO temperature-programmed desorption (CO-TPD) results showed that cobalt enhanced the adsorption and activation of intermediate CO on Na x Fe-Co catalyst, thereby promoting the catalytic conversion of CO 2 . The complexation of EDTA promotes the synergistic effect of Fe-Co bimetals, enhances the chemical adsorption of CO 2 . Sodium in EDTA-2Na promotes the surface basicity of the catalysts, which is favored for improving the product distribution of hydrocarbons. At lower H 2 /CO 2 (1/1) ratio, the EDTA-2Na modified Fe-Co/Al 2 O 3 catalyst exhibited high conversion of CO 2 (32.8 %) and excellent selectivity toward high value-added chemicals. The selectivity of by-product CO was only 8.1 %; and C 2 -C 4 = (32.5 %) and C 5 -C 11 (46.3 %) accounted for ∼79 % selectivity among the hydrocarbons generated.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Carbon Capture Science & Technology
·
2021
·
IF 0
Yuxin Mei,Nicui Yuan,Yuwei Liu,Xin Zhang,Baining Lin,Yonghua Zhou
Boron carbon nitride (BCN) is an emerging metal-free catalyst for CO 2 photocatalytic reduction. However, the fast electron-hole recombination as well as the weak absorption for ultraviolet-visible (UV-vis) light are still challenging for the activity upgrading of BCN. In this paper, a BCN/CeO 2 heterostructure via N-O-Ce bonding was fabricated by a urea-assistant heat-precipitation technique and confirmed by XRD, FT-IR, SEM, TEM and XPS characterizations. For CO 2 photoreduction with H 2 O as reducing agent, the BCN/CeO 2 heterostructure delivered an obviously enhanced catalytic performance with CO yield of ca. 6-fold that of BCN. UV-vis diffuse reflectance spectrophotometer (DRS), electrochemical impedance spectroscopy (EIS) and transient photocurrent response measurements revealed that the electron-hole separation efficiency and charge transfer are efficiently promoted on CeO 2 /BCN heterostructure, along with the boosted light harvesting in visible and ultraviolet light range. Furthermore, based on the photo(electro)chemical and photocatalytic results, a possible CO 2 photocatalytic reduction mechanism was proposed.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
DOI
JOURNAL OF APPLIED PHYSICS
·
2022
·Vol. 132
·期 18
·
IF 2.877
Zheng Xiaochun,Ren Shoutian,Gai Qixiao,Wang Yidi,Liu Wenjun
Various defects of nanocomposites inevitably bring some harmful effects on their photoelectric performance, especially considering that interface defects seriously hinder the carrier interfacial transfer. Here, the interface optimization can be realized between graphitic carbon nitride (C 3 N 4 ) and CoP co-catalyst by the introduction of good conductive carbon nanosheets (CNs). As a result, the defect density of synthesized C 3 N 4 /CNs/CoP is reduced to 1.40 × 10 12 cm −3 from 2.55 × 10 12 cm −3 of C 3 N 4 /CoP, and its interface impedance is correspondingly reduced to 34% of that of C 3 N 4 /CoP. Therefore, the optimal H 2 evolution rate of 5.26 mmol g −1 h −1 and apparent quantum efficiency of 9.27% at 420 nm are realized, which are 4.8 and 8.1 times that of C 3 N 4 /CoP photocatalyst in the absence of CNs, respectively. This work provides a general solution to reduce defect density and carrier transfer resistance in nanocomposites by the introduction of a highly conductive buffer layer.
研究领域:
材料科学
·
光催化
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2023
·Vol. 34
·期 20
·1-12
·
IF 2.8
Chen Yongzhi,Wen Xu,Zhang Xiaohong,Yang Chao,Wang Lihua,Zhou Lingfeng,Li Zuohong,Deng Haobo,Li Jian
The recycled graphite (RG) and a new type of recycled graphite with multi-layer coating structure (RGC) were prepared by using spent graphite and asphalt. The electrochemical properties and coatings of RG and RGC were also investigated. The low graphitization degree of hard carbon and soft carbon was beneficial to improve the electrochemical properties of regenerated graphite, which was verified by first principles. The unique structure (soft carbon/ hard carbon/ graphite) limited the volume expansion of hard carbon and graphite when lithium ions were embedded or extruded, which improved the rate capability and cycling performance of the battery. Compared with spent graphite (SG) and recycled graphite (RG), the first charge-specific capacity of RGC at 0.1 C was 349.17 mAh·g − 1 , and the coulombic efficiency was 82.47%. Impressive reversible capacity was 263.38 mAh·g − 1 after 130 cycles at 0.5 C and discharge capacity of 188 mAh·g − 1 at 1 C. Due to the pre-lithiation of RGC, the first coulomb efficiency (99.49%) of the full battery (18,650) was higher than that of commercial graphite, and the energy conservation rate was 65.6% after 2000 cycles. This study provides a simple and effective scheme, and realizes the clean recovery and high value commercial application of spent graphite.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Mingjun Cui,Yujie Qiang,Wei Wang,Haichao Zhao,Siming Ren
In this work, nitrogen doped carbon dots (NCDs) were prepared with citric acid monohydrate (CA·H 2 O) and ethanolamine (EA) via microwave method. In combination with electrochemical techniques, weight loss and SEM, it is found that nitrogen doping in carbon dots effectively suppresses the corrosion of Q235 carbon steel in HCl solution owing to the presence of pyrrolic N in NCDs. Especially for NCDs (1:10), the optimum inhibition efficiency is about 89% after 1 h of immersion in 0.1 M HCl solution with 500 ppm of concentration. By further calculation, the Δ G ads 0 value for NCDs (1:10) is -26.65 kJ·mol -1 , indicating the adsorption of NCDs on Q235 carbon steel surface involves both chemisorption and physisorption. In addition, NCDs still remain superior corrosion inhibition performance with the prolonged immersion time and ascending temperature.
研究领域:
材料科学
·
腐蚀与防护
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Fangqi Yang,Chang Jiang,Mingfeng Ma,Fenghao Shu,Xinyu Mao,Weikang Yu,Jun Wang,Zheling Zeng,Shuguang Deng
Electrochemical reduction of CO 2 into formic acid (HCOOH) is an appealing approach to mitigate the CO 2 emission problem and achieve a carbon-neutral cycle but remains a challenge. Herein, we present a novel strategy to prepare Cu nanoparticles embedded in carbon substrate (Cu NPs@C) as efficient CO 2 reduction reaction electrocatalysts for highly selective HCOOH production. The uniformly distributed Cu nanoparticles are responsible for the high faradaic efficiency of HCOOH of 78% at −1.0 V (RHE) and yield of 82.8 μmol h −1 cm −2 at −1.2 V (RHE). Moreover, the detailed density functional theory (DFT) calculations have demonstrated that the high activity and selectivity for HCOOH production was attributed to the synergy effects of exposed Cu (111) facets and carbon substrate. The charges transferred from Cu induces a charge-rich environment on the carbon surface, which enhances the *OCHO adsorption and boosts the HCOOH formation. This work paves a new way to synthesize novel Cu-based electrocatalysts for efficient production of HCOOH.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 49
·期 3
·746-754
·
IF 2.7
Bing Fang,Haiyue Wang,Wei Chang,Yibang Yao,Liying Guo,Yuanyuan Zhao,Bing Liu
The utilization of aliphatic diols as a substitute for epoxides in the reaction with CO2 to produce cyclic carbonates offers a cost-effective and less hazardous synthesis route. This approach aligns with green chemistry principles and presents new strategies to combat climate change. This study primarily focuses on the innovative application of an alkaline ionic liquid in conjunction with a Brønsted acid for the catalytic synthesis of cyclic carbonates from CO2 and aliphatic diols. Three alkaline ionic liquid catalysts [DBUH]PHY, [TBDH]PHY, and [DBUH]TBD were successfully synthesized using 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD), and phenol as precursors. Their chemical structures and thermal properties were systematically characterized using Fourier-transform infrared spectroscopy (FT-IR), proton nuclear magnetic resonance (1H-NMR), carbon nuclear magnetic resonance (13C-NMR), and thermogravimetric (TG) analysis. The catalytic performance of the three alkaline ionic liquids combined with various Brønsted acids (including sulfuric acid, phosphoric acid, and acetic acid) for the synthesis of ethylene carbonate (EC) from ethylene glycol (EG) and CO2 was investigated. The results demonstrated that the combination of [DBUH]PHY with sulfuric acid (H2SO4) exhibited the best synergetic catalytic effect. Subsequently, the process parameters were optimized to study the effects of reaction temperature, pressure, time, and catalyst loading on catalytic performance. Under optimized conditions, the catalytic efficiency of [DBUH]PHY and sulfuric acid in the synthesis of cyclic carbonates from different aliphatic diols, including ethylene glycol, propylene glycol (1,2- and 1,3-), and butanediol (1,4-), was explored. This study successfully achieved the activation of aliphatic diols and CO2 through cooperative catalysis of alkaline ionic liquids and Brønsted acids, providing an innovative catalytic system for research in this field.
研究领域:
化学
·
环境科学
✓ 已验证
DOI
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2021
·
IF 8.528
Hanxiong Lyu,Naiyu Jiang,Yingze Li,Dongxing Zhang
The weak interfacial adhesion caused by the low wettability of carbon fiber (CF) and inert polyetheretherketone (PEEK) hinders the great application potential of CF/PEEK composites. In this study, the interface between CF and PEEK was modified by coating hydroxylated PEEK grafted onto multi-walled carbon nanotubes (M-HPEEK). Modified CFs by M-HPEEK sizing had rougher surfaces with more polar groups, showing decreased contact angle and increased surface energy. The wettability of these CFs was enhanced, beneficial to PEEK infiltration and physical adhesion improvement. As a result, the interlaminar shear strength , flexural strength , and flexural modulus of modified CF/PEEK composites were increased by 73.0% (84.7 MPa), 163.2% (906.2 MPa), and 84.8% (58.4 GPa), respectively. An improved interface with stress transferring was proved by the interface debonding failure changed to fiber crack and resin yield. M-HPEEK sizing is considered as a promising modification method to optimize the interface performance of composites.
研究领域:
材料科学
·
复合材料工程
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Huahua Zhao,Huanling Song,Fangyuan Wang,Zhichao Miao,Lingjun Chou
In the present work, a new strategy was developed to fabricate strong basicity on mesoporous zirconia by in-situ preservation of carbon species originated from organic template during the thermal treatment of mesoporous ZrO 2 . The carbon species was maintained on mesoporous zirconia by calcination in N 2 prior to the introduction of base precursor KNO 3 . The decomposition temperature of KNO 3 to strongly basic site K 2 O was significantly reduced from higher than 650℃ to about 400℃ in the presence of carbon species, which fascinatingly converted the endothermic decomposition reaction to exothermic process. More importantly, the tetragonal ZrO 2 support with excellent mesostructure was well stabilized by the carbon species after introduction of K species. Therefore, K 2 O supported on mesoporous tetragonal zirconia (K 2 O/M-ZrO 2 -C) were successfully fabricated. The resultant mesoporous basic material presented good activity in the synthesis of dimethyl carbonate (DMC) and the DMC yield was 60.0 %, apparently higher than that (18.1 %) of the catalyst prepared without preserving carbon species (K 2 O/M-ZrO 2 ). The strong basicity and the uniform mesopores of the catalyst were suggested to be contributed to the high activity. The obtained results will provide some fundamental understanding and guidance for rational catalyst design.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Mengxue Zhang,Liheng Xu,Changli Qi,Ming Zhang
To improve the removal efficiency of pharmaceutical antibiotics from water by adsorption technologies, it is vital to optimize the porous geometrical structure of carbonaceous adsorbents. In this study, a hierarchical porous carbon that possesses micro/meso bimodal pores (MMC) is synthesized and is employed in the adsorption of tetracycline in both batch mode and column mode. In comparison, microporous carbon, mesoporous carbon, and commercial activated carbon (AC) are induced as carbonaceous adsorbents. In batch mode adsorption, the maximum adsorbed amount of tetracycline on MMC reaches 701.31 mg/g, which is twice as much as that on AC. While in the column adsorption process, the treatment capacity and the total adsorbed amount of MMC toward tetracycline are found 10 times greater than those of AC. The porous geometrical structure of the adsorbent is revealed to play an important role in determining the adsorption efficiency in the column adsorption process with a limited contact time. The surface utilizations of MMC in the column process keep similar to that in batch adsorption, which is totally different from the remarkable decreases in other studied adsorbents. The specific bimodal porous structure of MMC benefits the full play of its adsorption potential in column operation. The channel-like mesopores of MMC are helpful in providing a low resistance for the rapid transport of tetracycline molecules, and the micropores further enhance the accessibility and availability of adsorption sites.
研究领域:
环境科学
·
材料科学
·
水处理
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xue Zhao,Xue Li,Haibo Zhang,Xiao Chen,Jian Xu,Jun Yang,Hucai Zhang,Guangzhi Hu
Environmentally friendly electrochemical reduction pathways from NO 3 − to NH 3 or N 2 have provided feasible strategy into the green production of ammonia or the treatment of nitrate wastewater. Here, we anchored single-atom Cu with boron carbon nitride on carbon nanotube (BCN@Cu/CNT), and achieved the efficient operation of electrochemical nitrate reduction reaction (NIRR). BCN@Cu/CNT can efficiently catalyze the selective conversion of high-concentration nitrate into high-value-added ammonia, where the ammonia yield rate and Faradaic efficiency are as high as 172,226.5 μg h −1 mg cat. −1 and 95.32% (at −0.6 V), respectively. BCN@Cu/CNT also shows the ability to efficiently remove low-concentration nitrates in sewage. Specifically, here only takes 5 h to nearly 100% (99.32%) eliminate NO 3 - (50 mg L −1 ) in sewage without any residual NO 2 − . The excellent catalytic activity and physicochemical stability of BCN@Cu/CNT for NIRR suggest the promising industrial application prospects, including the green production of ammonia and the purification of nitrate wastewater.
研究领域:
环境科学
·
电化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 9
·3270-3278
·
IF 6.119
Huihui Li,Fuchun Ning,Xiaofei Chen,Anye Shi
Porous carbon nitride nanosheets with carbon and nitrogen double vacancies have been synthesized by a soft template-supported one-pot method. Besides their highly defined and unambiguous structure, they also show minimal thickness and high crystallinity. This porous carbon nitride exhibits great enhancement in photocatalytic hydrogen evolution activity (297.6 μmol h−1), which is 9.6 times higher than 31.2 μmol h−1 of the pristine one. An apparent quantum yield of 12.7% at 420 nm for hydrogen production can be achieved over these porous nanosheets. The detailed investigation suggests that there are carbon vacancies along with nitrogen vacancies. Besides nitrogen vacancies, carbon vacancies also play a positive role in the improvement of hydrogen evolution. In addition, the photocatalytic performance especially hydrogen evolution increases with the increase of the C/N ratio.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）