POWDER TECHNOLOGY
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2023
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IF 5.2
Duanlian Tang,Xiaoying Lyu,Zhixian Huang,Renwei Xu,Jie Chen,Ting Qiu
Nitrogen-doped microporous carbon, which features a uniquely tunable porosity, exhibits promisingly high adsorption prospects in the greenhouse gas capture and water treatment. Herein, we propose a series of novel N-doped microporous carbons (CMPA n -C1000), and precisely tune their porosities via a direct pyrolysis of rigid conjugated microporous poly(aniline)s (CMPA n , n = 1, 2, 3) with pore size difference in a molecular level, as achieved by simply tuning their linkers with varying sizes, planarity, and symmetry. The CMPA3-C1000, with a satisfactory amount of nitrogen heteroatoms , high S BET of ∼800 m 2 g −1 , and large ultra-micropore volume of 0.25 cm 3 g −1 , has excellent CO 2 capture ability ( i.e. , 5.1 mmol g −1 at 273 K, 1 atm) and Hg(II) adsorption performance ( i.e. , Q e = 571 mg g −1 ; k 2 = 0.0031 g mg −1 min −1 ), respectively. CMPA3-C1000 might perform chemisorption towards Hg(II), according to calculations using density functional theory and experimental data; nitrogen atoms in porous carbon contributed to this excellent Hg(II) adsorption.
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International Journal of Applied Ceramic Technology
·
2023
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IF 2.1
Fangyi Huang,Xiaoli Tang,Qin Zhang,Xingyu Huo,Yuanxun Li,Xian Jian,Hua Su
In this study, the microwave dielectric properties of Co 2+ -substituted BaZnP 2 O 7 ceramics prepared through conventional solid-state synthesis were investigated. X-ray diffraction, Rietveld refinement, energy-dispersive spectroscopy, and Raman spectroscopy all indicated that BaZn 1− x Co x P 2 O 7 ceramics sintered at 875°C were composed of a single phase. The lattice strain and crystallite size were estimated using Williamson–Hall (W–H) method. Both the scanning electron microscopy images and density measurements showed that Co 2+ ions had an effect on the grain growth and densification of ceramics. The microwave dielectric properties were influenced by the intrinsic and extrinsic factors that varied with the increase of x value. An optimal performance ( ε r = 7.62, Q × f = 600 45 GHz, and τ f = −74 ppm/°C) was achieved at x = .01. The porosity and relative density played a significant role in the dielectric constant ε r : the denser the ceramic structure, the larger the dielectric constant. The Q × f and τ f values were negatively correlated with the full width at half maximum of the Raman vibrational peak at approximately 1049 cm −1 . Moreover, the Q × f value was improved compared to that of the undoped BaZnP 2 O 7 ceramics. Therefore, cobalt ion substitution is an effective strategy to enhance the performance of microwave dielectric ceramics.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xiaohong Ma,Danyang Li,Huacheng Jin,Xi Zeng,Jian Qi,Zongxian Yang,Feifei You,Fangli Yuan
Herein, an urchin-like Fe 2 O 3 @In 2 S 3 hybrid composite is designed and synthesized using a facile process. The composite efficiently harvests light in both the ultraviolet and visible regions, and the unique hierarchical structure provides several advantages for photocatalytic applications: (i) a suitable band-matching structure and broadband-light absorbing capacity enable the reduction of CO 2 into hydrocarbon, (ii) the extensive network of interfacial contact between nano-sized Fe 2 O 3 and In 2 S 3 significantly increases the separation of charge carriers and enhances the utilization of photogenerated electron-hole pairs, and (iii) an abundance of surface oxygen vacancies provide numerous active sites for CO 2 molecule adsorption. The optimized Fe 2 O 3 @In 2 S 3 composite generated CO from the photocatalytic reduction of CO 2 at a rate of 42.83 μmol·g −1 ·h −1 , and no signs of deactivation were observed during continued testing for 32 h under 300 W Xe lamp irradiation.
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PubMed
高影响因子
CARBON
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2022
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IF 11.307
Hui Cao,Yumeng Yan,Yuan Wang,Fei-Fei Chen,Yan Yu
The activity of photocatalytic CO 2 reduction (PCR) remains inadequate due to the thermodynamically stable CO 2 molecules and sluggish carrier kinetics. This work simultaneously adopts active site and heterojunction engineering to collaboratively enhance PCR. A heterojunction of g-C 3 N 4 microtube-supported Co 3 O 4 nanoparticle has been developed through the hydrothermal pretreatment and calcination processes. The g-C 3 N 4 microtubes play dual roles in enhancing PCR of Co 3 O 4 : (1) they act as a substrate to support Co 3 O 4 nanoparticles, thereby making small size and good dispersion of Co 3 O 4 nanoparticles. The Co active sites can be highly exposed to accept photogenerated electrons and capture CO 2 molecules; and (2) the p-type Co 3 O 4 nanoparticles and n-type g-C 3 N 4 microtubes build a p–n junction. An internal electric field is created to expedite the charge transfer. As a result, the g-C 3 N 4 microtube-supported Co 3 O 4 nanoparticle affords a significantly high turnover number (TON) of 24.72, which is 24-fold higher than that of the pure Co 3 O 4 and comparable to state-of-the-art photocatalysts .
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Journal of Physical Chemistry C
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2022
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IF 4.177
Xudong Wu,Ruijie Xu,Xianli Li,Ruosheng Zeng,Binbin Luo
As a potential candidate for photocatalytic CO2 reduction, CsPbX3 perovskite nanocrystals (PNCs) have attracted enormous attention due to their suitable energy band structure and large molar extinction coefficient for visible light. However, the catalytic performance on CO2 reduction is greatly limited due to the intrinsically fast radiative recombination and poor stability of PNCs. In this work, PbS nanoparticles are uniformly anchored on CsPbBr3 PNCs with the assistance of a bridged amino acid due to the directed interaction between −COO– (−NH3+) and Pb2+ (Br–). Because of the small lattice mismatch between PbS and CsPbBr3, the introduction of PbS significantly quenches the emission of CsPbBr3 and boosts the interfacial charge transfer, thereby resulting in an enhanced photoelectrocatalytic CO2 reduction rate of ∼2.94 and 0.36 μmol cm–2 h–1 for CO and CH4 products, which are ∼2.4 times higher than that of pristine CsPbBr3 PNCs, respectively. This work provides a universal strategy of constructing homogeneous nanocomposites for catalytic applications.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Yanzhao Wu,Xiaoyang Yue,Jiajie Fan,Xiaoming Hao,Quanjun Xiang
In recent years, the semimetal bismuth with surface plasmon resonance (SPR) effect has attracted great attention due to its application in enhancing photocatalytic activity. Herein, we developed a novel plasma-enhanced Bi/CsPbBr 3 composite photocatalyst by in situ growth method (BCPB-IS) using the fabricated CsPbBr 3 nanosheets (CPB) as the substrate for subsequent growth of Bi nanoparticles. Without the addition of any sacrificial agent, the CO yield of BCPB-IS reaches 76.4 µmol g −1 with an over 97% selectivity of CO under 4 h visible light irradiation. Such remarkable CO 2 reduction activity far exceeds that of pure CPB. The enhanced activity can be attributed to these factors: (1) The SPR effect from the loading of Bi NPs enhances the light response performance of BCPB; (2) The simultaneously generated hot electrons leads to rising ambient temperature, which promotes the electron transfer efficiency and photoreduction reaction efficiency; (3) The energy band bending effect at the interface of BCPB further improves the carrier separation and transfer performance. The enhanced separation and transfer performance of photogenerated carriers were investigated in detail by X-ray photoelectron spectroscopy (XPS), Infrared thermograms and Time-resolved photoluminescence spectra (TRPL).
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Journal of Materials Chemistry A
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2022
·Vol. 10
·期 42
·22468-22476
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IF 14.511
Guilin Yin,Xiaosi Qi,Yanli Chen,Qiong Peng,Xingxing Jiang,Qinglong Wang,Wenhua Zhang,Xiu Gong
Metal halide perovskite quantum dots (QDs) are regarded as one of the promising photocatalysts for CO2 reduction because of their unique optoelectronic properties. However, severe charge recombination and insufficient CO2 absorption/activation have limited photocatalytic CO2 reduction. Herein, we report an efficient 0D/0D CsPbBr3/CdSe heterojunction consisting of CdSe QDs in situ grown on CsPbBr3 QDs for high-performance photocatalytic CO2 reduction using water as the electron donor in organic solution. The type-II 0D/0D heterojunction with the strong electronic coupling of Pb–Se and Br–Cd bonds between CdSe and CsPbBr3 facilitates fast electron transfer. Moreover, the specific abundant edge- and corner-sites of CdSe accelerate the CO generation by forming a Cd–C2O4− adduct, enabling superior CO2 activation capacity and efficient CO2 conversion into CO. Consequently, assisted by water to provide electrons and protons, the yield of main product CO reaches 115.26 μmol g−1, which is 4.6-fold higher than that of pristine CsPbBr3. This study is expected to provide a new way to fabricate high-performance perovskite-based catalysts in the field of photocatalysis.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yunhan Bai,Xiaoshu Ding,Ying Sun,Yucong Song,Yanji Wang
The reverse water gas shift (RWGS) reaction is one kind of the catalytic conversion of CO 2 to reduce an enormous amount of CO 2 . However, the RWGS reaction has the safety hazards associated with the use of hydrogen and thermodynamic limitation. Therefore, this work proposes a new safe and efficient reaction route (CO 2 -MCH) to get CO from CO 2 and methylcyclohexane (MCH). Thermodynamic calculations showed that the equilibrium CO 2 conversion at 350 °C increased from 17.8 % of the RWGS reaction to 53.5 % of the CO 2 -MCH reaction. In the CO 2 -MCH reaction, the relationship of the catalytic performance with the metal dispersion, the Pt particle size and the acidity of Pt-based catalysts on the different supports was investigated, respectively. The results showed that the Pt/γ-Al 2 O 3 catalyst with high dispersion of Pt particles, small particle size and medium acidity had good activity and selectivity. The relationships among Pt loading and Pt particle size on the Pt/γ-Al 2 O 3 catalyst and the catalytic performance were evaluated. The Pt particle size gradually increased with the metal loading. A positive correlation was observed between Pt particle size and CO 2 conversion; a volcano-type relationship was observed between CO selectivity and Pt particle size. In the CO 2 -MCH reaction at 350 °C, 0.1 MPa, LHSV = 6 h −1 , the CO 2 conversion was 24.7 %, the CO selectivity reached 95.2 %, and the Pt/γ-Al 2 O 3 catalyst within 40 h showed good stability. Moreover, the mechanism of the CO 2 -MCH catalytic reaction over the Pt/γ-Al 2 O 3 catalyst was speculated.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wenchuan Jiang,Wenrui Liu,Yunpeng Wang,Zhiyu Zhao,Qing Li,Yifan Wu,Tao Liu,Heping Xie
Electrochemical CO2 capture driven by a proton-coupled electron transfer (PCET) reaction, exploiting the CO2 hydration/dehydration equilibrium through pH swing, has the potential for low-energy capture as it eliminates the sensible heat from the temperature-swing process. However, carbonate salts used in the pH swing method suffered from poor reaction kinetics and crystal accumulation, which could potentially clog electrodes and become electrically disconnected. While amines are widely applied in various methods as efficient capturing agents, their capture energy consumption is generally higher than 100 kJ/mol CO2. Here, we propose a scheme of electrochemical CO2 capture driven by a PCET reaction using amines instead of carbonates as CO2 capture agents. In this scheme, H+ generated by the PCET reaction will promote CO2 desorption from the amine–CO2 compound, and the CO2 absorption of amines can be achieved through the consumption of H+ by the PCET reaction. Furthermore, we establish a thermodynamic model of the energetic cost of the method by introducing a multibuffer system of amines, showing that the introduction of amines will moderate the pH swing during the four-stage cycle, resulting in a 45.2% reduction in theoretical CO2 capture energy consumption compared to carbonate. Besides, we validated the model and obtained an experimental energy cost of 21.0 kJe/mol with 0.15 bar CO2 (g) captured using a hydrogen cycle. We expect that this strategy of introducing a multibuffer system to reduce CO2 capture energy consumption could provide a reference for low-energy consumption electrochemical CO2 capture in the future.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zhuoran Ren,Fang Chen,Qin Zhao,Guoqiang Zhao,Hui Li,Wenping Sun,Hongwei Huang,Tianyi Ma
Piezocatalysis has attracted the increasing interest of researchers as a novel catalytic method. To date, there are two popular mechanisms regarding the piezocatalysis, i.e., the piezoelectric effect and the energy band theory. However, both mechanisms cannot fully explain the piezocatalytic process: the electrons generated by the piezoelectric effect will not spontaneously participate in the piezocatalysis, while not all piezoelectric materials have an appropriate energy band structure. In this work, displacement current and the principle of piezoelectric nanogenerator are introduced to fully comprehend the piezocatalytic mechanism for the first time. As a proof-of-concept catalytic system, we synthesize Co-N-C@BaTiO 3 piezocatalyst for the CO 2 reduction reaction (CO 2 RR) under ultrasonic vibration. A promising piezocatalytic CO 2 reduction rate of 261.8 mol g −1 h −1 is achieved with a high CO selectivity up to 93.8% under 50 kHz ultrasonic vibration. The CO yields of this catalytic system outperform most of the reported photocatalytic CO 2 RR and piezocatalytic CO 2 RR. Moreover, a comprehensive piezocatalytic mechanism from displacement current to active sites is proposed and supported by combining Co-N-C@BaTiO 3 piezoelectric nanogenerator, COMSOL simulation and energy band structure analysis. Under the ultrasonic vibration, the electrons generated by the piezoelectric effect are driven by the time-varying electrostatic potential formed by the displacement current. The suitable band structure of piezoelectric provider that satisfies the potential of reaction promotes electrons to participate in CO 2 RR on active sites. Overall, our work provides an insightful understanding of piezocatalysis and paves a new path for its development.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Cong Jiang,Maohong Fan,Ge Gao,Wufeng Jiang,Xiaoshan Li,Cong Luo,Liqi Zhang,Fan Wu
In order to alleviate the intensive energy demand of amine-based post-combustion carbon capture technology, metal oxyhydroxide AlOOH of nanoscale was synthesized through the hydrothermal method and applied to accelerate the CO 2 desorption rate and reduce the regeneration heat duty of aqueous monoethanolamine (MEA) solution for the first time. Results showed that the use of AlOOH could accelerate the desorption rate by up to 560% and increase the desorption amount by 251%. By comparing the performance between AlOOH and Al 2 O 3 , it can be found that the presence of extra hydroxyl groups is 20.6% more efficient in catalyzing CO 2 desorption. According to a simplified heat transfer model created in this work, AlOOH could reduce the heat duty by 17% with only 0.1 wt% loading, which exhibited the highest performance cost ratio among related literature. In addition, the cyclic stability of AlOOH was confirmed through various characterization methods, including XRD, FT-IR, SEM, and N 2 adsorption–desorption. More importantly, a possible catalytic mechanism of AlOOH was discussed and proved where it could change reaction pathways in different CO 2 loading regions. This work reveals a promising research direction towards cost-efficient and high-performance metal oxyhydroxide catalysts in the catalytic amine regeneration field to approach the net-zero carbon emission goal.
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JOURNAL OF CATALYSIS
·
2022
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IF 8.047
Jing Huang,Jiawei Dai,Jiannan Zhu,Rong Chen,Xiaoqi Fu,Hongfang Liu,Guangfang Li
Electrocatalytic reduction of CO 2 (CO 2 RR) represents a promising approach to reduce CO 2 emission and generate value-added chemicals. Herein, we developed bimetallic Au-Cu gradient alloy nanostructures (AuCu-g) comprising of ultrathin Cu-rich alloy surface and Au-rich alloy core as electrocatalyst via a facial solvothermal method. Impressively, the AuCu-g can stably generate a considerable amount of C 2 H 4 with faradaic efficiency (FE) ∼20 % at a low limiting potential of −0.4 V versus reversible hydrogen electrode (RHE) due to its unique gradient structure and multi-component tandem effect. The potential-dependent in situ Raman spectrum indicated an enhanced *CO adsorption strength and a remarkable CO intermediate generation over Au-Cu gradient alloy at low overpotentials during CO 2 reduction process. This work shines a light for developing mutilmetallics toward efficient CO 2 RR.
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