Materials Today Sustainability
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2022
·
IF 7.244
R. Zeng,G. Jin,D. He,L. Zhang,D. Chen,Y. Zhang,L. Zhu,Y. Mei,W. Wu,Y. Luo
Utilizing propane and CO 2 as coreactants to produce syngas (CO/H 2 ) via dry reforming shows several advantages over direct propane dehydrogenation and traditional methane dry reforming . It is of great importance to establish high-efficiency catalytic systems that can break C–C bonds and activate CO 2 simultaneously. Herein, acidic H 2 O 2 was applied to etch LaCoO 3 . Surprisingly, highly dispersed Co 3 O 4 at the edges of support along with high oxygen vacancies were obtained from acidic H 2 O 2 treatment. Furthermore, the treated LaCoO 3 catalyst facilitated the generated intermediates of formate to convert into the desired products. The results showed that acidic H 2 O 2 treated LaCoO 3 catalyst can reach 18% for propane conversion and 35% for CO 2 conversion at 550 °C, showing high catalytic activity . Consequently, the present work provides some ideas for the synthesis of efficient LaCoO 3 catalysts for dry reforming of propane.
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Materials Today Energy
·
2022
·
IF 9.257
Xinxin Bian,Bowen Liu,Xiaolei Wang,Zhimin Chen,Rui Gong,Wanqi Jia,Zichen Song,Huiyuan Meng,Weibo Yin,Zhiyu Ren
Defects engineering is one of the effective strategies to advance the CO 2 conversion into value-added chemicals and fuels during the electrochemical process. It is noteworthy that multiple defects are often associated in the reaction process, hence how to stimulate their synergistic effect is extremely important, but still lacks in-depth understanding. Herein, SnO 2 nanosheets with simultaneous oxygen vacancies and Zn dopants (Zn–Vo–SnO 2 ), as a proof-of-concept study, were proposed to elucidate the synergistic effect of multiple defects on enhanced CO 2 -to-C 1 conversion. Zn–Vo–SnO 2 , which is prepared by coupling a facile hydrothermal reaction and a subsequent desulfurization, yields the C 1 products at the lower applied potential, and maintains the FE C1 of about 95% at −0.80 V vs. RHE for a long-term operation. Evidences from systematic experiment and theoretical calculation corroborate that the charge redistribution caused by the oxygen vacancies and Zn-doping synergistically energize the CO 2 conversion, in the term of the CO 2 adsorption, the hydrogenation of CO 2 and intermediates, and the thermodynamic energies of the rate-determining steps. This study has an insight into defect engineering to design advanced electrocatalysts for implementable CO 2 recycling and utilization.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Rui Li,Jenaidullah Batur,He Bian,Ying-Jie Wang,Zunbin Duan,Yabo Xie,Jian-Rong Li
Photocatalyzed CO2 reduction (CO2RR) transfers CO2 into valuable products using renewable energy, attracting widespread attention. Composite catalysts fabricated with TiO2 and red phosphorus (RP) might exhibit competitive advantages, but effective interphase binding is difficult to forge. The composites therefore require complex and energy-consuming syntheses, severely hindering their application in CO2RR. In this work, TiO2/RP composites with hyperefficient interphase contact, which outperform various elaborately designed catalysts, are directly prepared from commercially available materials via a green and facile hydrothermal approach. The low heating temperature and sole solvent of water diminish the energy input for synthesis and imply a potential opportunity to propel CO2RR with industrial waste heat and cooling water. Experimental and computational analyses reveal that hydrothermal synthesis reduces the interfering oxidized species on the exterior surface of RP, facilitating the relatively less favored interphase contact between TiO2 and nonoxidized RP. Photoelectron transfer and catalytic performance of the composites are hence drastically enhanced. Further improvement of activity is feasible by slightly elevating the heating temperature, time, or solution acidity. Attributing to the universal applicability of this green approach, different metal oxide/RP composites (e.g., WO3/RP) are similarly prepared, consistently boosting the reaction rate multiple times.
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ACS Applied Nano Materials
·
2022
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IF 6.14
Yue Liu,Xukun Zhu,Ling Qin,Tong Zhang,Shuhan Wang,Yachao Jin,Li Song,Ming-Dao Zhang
The construction of special heterogeneous interface structures without precious metals is found to be efficient for the development of low-cost and high-activity hydrogen evolution reduction (HER) catalysts. Here, we report a moderate method to develop an efficient and stable HER electrode especially composed of the Co2(OH)2CO3 (COC) nanowire substrate modified by benzenehexol (HOB) molecules. This kind of interfacial structure leads to prominent electrocatalytic HER performance in an alkaline environment with a low overpotential of 130.8 mV at a current of 20 mA cm–2. Meanwhile, density functional theory (DFT) calculations reveal that the nanoscale synergistic interfacial mechanism and strong electron interaction between HOB and COC can reduce the activation energy for HER.
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Solar RRL
·
2022
·Vol. 6
·期 10
·2200536
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IF 9.173
Rui Zhang,Linjia Li,YinYin Li,Dejun Wang,Yanhong Lin,Tengfeng Xie
CsPbBr 3 perovskite exhibits potential application in photocatalytic CO 2 reduction into valuable chemical fuels; however, enhancing carrier separation capability of the CsPbBr 3 and fully understanding the CO 2 reduction reaction process are still imperative. Herein, a new series of x SnS 2 /CsPbBr 3 nanocrystals (NCs)- y heterostructures are developed, which exhibit better catalytic activity in comparison with pure CsPbBr 3 NCs. Interface and surface carrier dynamic investigation reveals that this heterojunction structure can effectively improve carrier separation efficiency. Based on the interfacial electric field direction of CsPbBr 3 to SnS 2 , it is suggested that SnS 2 /CsPbBr 3 NC heterostructure satisfies Z-scheme transfer dynamics. Meanwhile, by the aid of in situ surface photovoltage, it is experimentally confirmed there is dynamic carrier interaction between CO 2 molecules and the SnS 2 /CsPbBr 3 NCs photocatalyst under irradiation, and a photocatalytic CO 2 reduction mechanism is thus proposed. This work expands the awareness of the interaction between CO 2 and the photocatalyst, which can be strongly influenced by carrier separation efficiency at the photocatalyst heterojunction.
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JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 32
·15474-15487
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IF 4.682
Liu Jiaxin,Qi Fei,Zhang Nan,Yang Jiayu,Liang Zhiyu,Tian Changqing,Zhang Wenxia,Tang Xiaosheng,Wu Daofu,Huang Qiang
Exploring novel and efficient photocatalysts to accelerate CO 2 photoreduction into useful chemicals or fuels is of great significance. In this work, we developed the three-dimensional (3D) structural heterojunction photocatalysts composed of ReS 2 and Cu 2 O by a drop-casting approach. The ReS 2 microspheres with nanosheets were deposited on the 3D structure of Cu 2 O/Cu foams. The analysis of UV–Vis absorption and PL spectra showed that the ReS 2 @Cu 2 O/Cu heterostructure delivered enhanced visible light absorption and improved charge carrier separation. The resulting ReS 2 @Cu 2 O/Cu-180 exhibited the CO yield of 14.3 µmol g −1 under the visible light irradiation. The realized S-scheme heterostructure not only promoted the separation of the photogenerated electron and hole pairs, but also enhanced the visible light absorption. Furthermore, the enriched electrons with high reducing abilities aggregated into the conduction band and diffused to the surface of Cu 2 O for favoring the CO 2 reduction and CO formation. This study is expected to provide a strategy to prepare high-performance S-scheme photocatalysts to perform efficient photocatalytic CO 2 reduction.
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Nano Research
·
2022
·Vol. 16
·期 3
·4152-4159
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IF 10.269
Yuan Xiaoqing,Liu Ju,Qin Jingyu,Ma Weili,Liu Guangyong,Wang Yanlei,He Hongyan
Stimuli-responsive materials have important applications in chemistry and chemical engineering. Here, we synthesized five different polyetheramine-fatty acids (PEFA) ionic liquids (ILs), possessing the dual stimuli-responsive ability to temperature and CO 2 . These PEFA ILs have reversible lower critical solution temperature (LCST) phase behavior over a wide temperature range of 37–91 °C, and reversible heterogeneous-homogeneous phase transition towards the addition and removal of CO 2 . Furthermore, the droplet size of the IL—water mixture system increased from 6.5 to 21.0 nm as the temperature increased from 25 to 56 °C, and then recovered to 6.5 nm when the temperature decreased to 25 °C. The addition and removal of CO 2 also reversibly modulated the droplet size of the system. Results from nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectra further showed that the temperature-dependent conformation of polyether amine chain in the cation dominates the temperature response, while the reversible formation of bicarbonate and fatty acids (FA) from CO 2 and anion controls the CO 2 -based reversible phase transition. Molecular simulations revealed a microscopic response mechanism of the IL—water system to temperature and CO 2 , and a synergistic effect between the dual stimuli of temperature and CO 2 . These findings may provide a basis for the rational design and understanding of ILs-based stimuli-responsive materials and nanoreactors.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Xinran Li,Shuohan Li,Jian Xu,Lanxin Wang,Kaiwei Liang,Huihui Zhang,Xuelian Yu,Zhongwei Liu
Photoconversion of CO 2 into fuel is critical for realizing a net-zero emission future, but it remains an open challenge due to the unsatisfactory light absorption and photogenerated carriers’ separation efficiency of catalysts. In this work, upon in situ thermal polymerization method, the nanodiamond (ND) are homogeneously and solidly modified on the defective graphitic carbon nitride (g-C 3 N 4 ) surface. Under visible light irradiation, the ND/g-C 3 N 4 (NH) exhibits excellent CO 2 photocatalytic performance with a CO yield of 10.98 μmol/h (18.6 times higher than bulk g-C 3 N 4 ), predominant performance in the selectivity of CO and cyclic stability. The improved CO 2 photoreduction ability was sourced from the synergetic effect of nitrogen vacancies engineering and ND decoration, which also significantly improved visible light absorption capacity and facilitated electron transport pathways, and promoted the separation and transfer of charge carriers efficiently.
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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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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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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
·
2021
·
IF 4.346
Azizullah Shaikh,Caili Dai,Yongpeng Sun,Qing You,Abdul Sami Qureshi,Guang Zhao,Varel Foutou,Allah Bakhsh,Nasir Khan,Zafarullah Abro,Mingwei Zhao
After the limitations of polymer-based fracturing due to poor clean-up property during flowback after fracturing treatment, viscoelastic surfactant (VES) received very huge attention in the last three decades, especially in low permeability reservoirs. In this study, a Novel CO 2 -induced clean fracturing fluid (SDS-TMTAD-CO 2 ) is formulated with simulated formation water (23,003 mg L −1 ) after optimization experiments according to the proposed parameters (i.e., 70 °C, economical, easily preparation, and environment-friendly). The results of rheological experiments show that the apparent viscosity of the fracturing fluid system increases to a certain extent under high salt conditions and possesses sufficient self-healing property against high shear tolerance. At different temperatures (25, 50, and 70 °C), the thermodynamic properties, fluid viscoelasticity, and proppant carrying capacity meet the requirements of the fracturing fluid industry standards. After adding kerosene (0.02 mol L −1 ); the gel breaking fluid viscosity (3.2 mPa s), anti-swelling rate (91.3%), and interfacial tension (2.3 × 10 −2 mN m −1 ) are holding promising conditions during the flowback period, clay swelling, and residual oil saturation, respectively. The filtration and core damage experimental results meet the national industry standard for fracturing fluids. The SEM results show that the fluid system after reaction forms a unified adsorption film on the core surface. Hopefully, this fluid system will be proved as a good candidate by means of excellent proppant transportation ability, anti-swelling, easy gel structure breaking, low filtration, and less formation damage in low permeable formations with an increase in productivity.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Xilu Hong,Zong Lu,Yali Zhao,Luxi Lyu,Li Ding,Yanying Wei,Haihui Wang
As one of the green, renewable, and clean energy resources, hydrogen is widely developed and utilized throughout the world. Highly efficient membrane separation for hydrogen production is required to give promising gas permeance with enough H 2 selectivity. The membranes are desired to be produced in large-scale, fast and facile methods. Here we report for the first time a kind of freestanding MXene-ZIF-8 dual-layered membrane for hydrogen separation. Fast synthesis of such membranes is realized by combining electrophoretic deposition (EPD) and fast current-driven synthesis (FCDS), achieving the assemble of MXene layer and growth of ZIF-8 layer, respectively, overcoming the traditional time-consuming vacuum filtration methods and solvothermal synthesis . The MXene-ZIF-8 dual-layered membrane prepared within 20 min exhibits significantly improved gas separation performance, whose H 2 /CO 2 selectivity increases from 44 for the pristine MXene membrane to 77 with H 2 permeance of 5.97 × 10 −8 mol m −2 s −1 Pa −1 . This concept of structure design of membrane can also be extended to other dual-layered membranes, including various 2D nanosheet layers combined with different MOF layers.
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