ADVANCED MATERIALS
·
2020
·Vol. 32
·期 24
·2000014
·
IF 27.398
Kai Feng,Shenghua Wang,Dake Zhang,Lu Wang,Yingying Yu,Kun Feng,Zhao Li,Zhijie Zhu,Chaoran Li,Mujin Cai,Zhiyi Wu,Ning Kong,Binhang Yan,Jun Zhong,Xiaohong Zhang,Geoffrey A. Ozin,Le He
The efficiency of heterogeneous photocatalysis for converting solar to chemical energy is low on a per photon basis mainly because of the difficulty of capturing and utilizing light across the entire solar spectral wavelength range. This challenge is addressed herein with a plasmonic superstructure, fashioned as an array of nanoscale needles comprising cobalt nanocrystals assembled within a sheath of porous silica grown on a fluorine tin oxide substrate. This plasmonic superstructure can strongly absorb sunlight through different mechanisms including enhanced plasmonic excitation by the hybridization of Co nanoparticles in close proximity, as well as inter- and intra-band transitions. With nearly 100% sunlight harvesting ability, it drives the photothermal hydrogenation of carbon dioxide with a 20-fold rate increase from the silica-supported cobalt catalyst. The present work bridges the gap between strong light-absorbing plasmonic superstructures with photothermal CO 2 catalysis toward the complete utilization of the solar energy.
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APPLIED CLAY SCIENCE
·
2020
·
IF 4.605
Xidong Du,Wenfeng Guang,Yugang Cheng,Zhenkun Hou,Zhenjian Liu,Hong Yin,Liang Huo,Ruide Lei,Couxian Shu
The greater adsorption ability of shale to CO 2 offers an alternative method to enhance shale gas recovery, where a potential solution for CO 2 sequestration into a deep shale reservoir can also be realized. Clay minerals are the important storage space for shale gas . In this work, the isotherm adsorption curves of CH 4 and CO 2 on montmorillonite at 288 K, 308 K and 328 K were obtained using gravimetric apparatus. The selectivity factor of CO 2 over CH 4 ( S CO2/CH4 ) and Henry's constants ( K H ) of CH 4 and CO 2 were calculated. More importantly, the thermodynamics parameters of CH 4 and CO 2 , including Gibbs free energy change (Δ G ), surface potential ( Ω ), isosteric heat of adsorption ( Q st ) and entropy change (Δ S ), were thoroughly analysed. The results indicate that all S CO2/CH4 values are obviously greater than one, and injecting CO 2 into a clay-rich shale reservoir to enhance the shale gas recovery is feasible. CH 4 has smaller K H than CO 2 , which shows that CH 4 has a weaker affinity on the montmorillonite surface. Low temperature helps to enlarge K H and promote the adsorption of CH 4 and CO 2 . Increasing the pressure causes the increase in Δ G and Ω of CH 4 and CO 2 . The higher Δ G and Ω of CO 2 compared to CH 4 reveal that the CO 2 adsorption on montmorillonite is more favourable and spontaneous. When the loading increases, the Q st values of CH 4 and CO 2 reduce. CH 4 has a smaller Q st than CO 2 , which suggests the stronger interaction of CO 2 with montmorillonite. CH 4 and CO 2 have decreasing Δ S with the loading. Under larger surface coverage conditions, the disorder of the adsorbed molecules is larger, and most of the injected molecules are trapped as a free state in the pore space . The higher ΔS of CO 2 illustrates that CO 2 molecules constitute a much more stable rearrangement than CH 4 molecules. The temperature has a slight effect on the Δ S of CH 4 and CO 2 .
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MOLECULES
·
2019
·Vol. 24
·期 20
·3732
·
IF 3.06
Li Ji,Zhonghui Qiao,Xin Zhang,Xiaolei Cheng,Weiyang Wang,Fan Zhang,Yifa Zhou,Ye Yuan
Monosialotetrahexosylganglioside (GM1) has good activity on brain diseases and was developed to be a drug applied in clinics for neurological disorders and nerve injury. It is difficult to isolate GM1 in industry scale from the brains directly. In this work, a simple and highly efficient method with high yield was developed for the isolation, conversion, and purification of GM1 from a pig brain. Gangliosides (GLS) were first extracted by supercritical CO2(SCE). The optimum extraction time of GLS by SCE was 4 h, and the ratio of entrainer to acetone powder from the pig brain was 3:1 (v/w). GM1 was then prepared from GLS by immobilized sialidase and purified by reverse-phase silica gel. Sodium alginate embedding was used for the immobilization of sialidase. Under the optimized method, the yield of high-purity GM1 was around 0.056%. This method has the potential to be applied in the production of GM1 in the industry.Keywords:ganglioside;GM1;supercritical CO2extraction;immobilization;sialidase;purification
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Pengju Shi,Xueqin Chen,Zhengguang Sun,Cao Li,Ziqiang Xu,Xueliang Jiang,Bingbing Jiang
Thickness controllable porous polymer nanofilm with superior gas storage capacity has gradually emerged as promising adsorbents for capture of CO 2 , due to extremely high surface area and micro-scale pore. In this work, we have developed a novel and facile strategy to fabricate thickness controllable two or three dimensional ordered porous nanofilm based on poly(styrene-butyl acrylate), in combination with covalently layer by layer (LBL) self-assemble process and hypercrosslinked post-treatment. Abundant microporous structures and a small number of mesoporous structures are formed in hypercorsslinked nanofilm and corresponding surface area derived from Brunauer-Emmett-Teller method (BET) were determined to be 605.7 m 2 /g. The capacity of CO 2 capture was also measured, which reach up to 53.6 wt% (12.2 mmol/g) at 273 K/1 bar, which is comparable to highest record. We have found that all the as prepared nanofilm with different thickness exhibited apparently enhanced micro- and meso-porosity after hypercrosslinking. Moreover, with the increase of thickness of nanofilm, the adsorption capacity decreases gradually, as well as the CO 2 adsorption capacity. An excellent recycling capacity for CO 2 capture have also found for this porous polymer nanofilm via repetitive adsorption-desorption assay. Our work confirmed that thickness controllable porous polymer nanofilm with superior CO 2 capture capacity can be fabricated by a very simple strategy which can meet the challenges of the current CO 2 capture and storage technology.
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Chemical Science
·
2019
·Vol. 10
·期 45
·10640-10646
·
IF 9.556
Jingjing Zhang,Qingli Qian,Ying Wang,Bernard Baffour Asare Bediako,Jiang Yan,Buxing Han
Currently, ethanol is produced via hydration of ethene or fermentation of foods. Lignin and CO2 are abundant, cheap and renewable feedstocks. Synthesis of ethanol using the lignin or its derivatives is of great importance, but is a great challenge and has rarely been reported. Herein, we propose a route to synthesize ethanol from CO2, H2, and lignin or various aryl methyl ethers, which can be derived from lignin. The reaction could be effectively conducted using Ru–Co bimetallic catalyst and the TON of ethanol could reach 145. Interestingly, ethanol was the only liquid product when lignin was used. A series of control experiments indicate that ethanol was formed via cleavage of aryl ether bond, reverse water gas shift (RWGS) reaction, and C–C bond formation. This protocol opens a way to produce ethanol using abundant renewable resources.
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ANNALS OF THE NEW YORK ACADEMY OF SCIENCES
·
2026
·Vol. 1563
·期 1
·e70406
·
IF 4.5
Yize Dang,Zilong Chen,Chengzhuang Zhang,Zhiqiang Han,Zinong Zuo,Kun Liang,Jia Fang
The rising concentration of greenhouse gases causes severe global warming, creating an urgent need for efficient and low-cost carbon dioxide (CO 2 ) adsorption technologies. Corn stover is an abundant agricultural waste that is often underutilized, leading to resource waste and environmental pollution. To develop value-added utilization of this material, corn stover−derived activated carbon is prepared via urea predoping and controlled potassium hydroxide (KOH) etching, while the effects of pyrolysis temperature, urea doping ratio, KOH dosage, and activation temperature are investigated. Under pure CO 2 at 25°C, the optimal adsorbent exhibits an equilibrium CO 2 adsorption capacity of 3.57 mmol·g −1 . Under pure CO 2 at 0°C, the equilibrium capacity increases to 5.91 mmol·g −1 , indicating that lower temperature favors CO 2 physical adsorption. Under a typical flue gas composition of 20% CO 2 /80% N 2 at 25°C, the adsorbent achieves a CO 2 uptake of 1.78 mmol·g −1 after 50 min. The adsorbent exhibits an ideal adsorbed solution theory CO 2 /N 2 selectivity of 30.92. The isosteric heat of adsorption ranges from 28.42 to 23.75 kJ·mol −1 . These values suggest predominantly physical adsorption on heterogeneous sites associated with nitrogen functionalities and structural defects. This study offers insights into the design of biomass-derived CO 2 adsorbents based on corn stover. Graphical Corn stover–derived activated carbon is prepared through urea predoping followed by KOH activation. Nitrogen functionalization and pore development provide complementary contributions to CO 2 capture. The optimized sample reaches 3.57 mmol·g −1 at 25°C and 5.91 mmol·g −1 at 0°C under pure CO 2 , and 1.78 mmol·g −1 after 50 min under simulated flue gas, with an ideal adsorbed solution theory CO 2 /N 2 selectivity of 30.92.
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Nano-Micro Letters
·
2023
·Vol. 16
·期 1
·1-17
·
IF 26.6
Wang Kangwang,Hu Zhuofeng,Yu Peifeng,Balu Alina M.,Li Kuan,Li Longfu,Zeng Lingyong,Zhang Chao,Luque Rafael,Yan Kai,Luo Huixia
The S-vacancies result in the change of d-band electronic state of Mo.
An internal quantum efficiency of 94.01% at 380 nm for photocatalytic CO 2 reduction reaction (CO 2 RR).
The Mo–S bridging bonds optimize adsorption energies and accelerate CO 2 RR kinetics.
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Materials
·
2023
·Vol. 16
·期 20
·6665
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IF 3.4
Manying Sun,Chuanwei Zhu,Su Wei,Liuyun Chen,Hongbing Ji,Tongming Su,Zuzeng Qin
Photocatalytic CO2reduction is a tactic for solving the environmental pollution caused by greenhouse gases. Herein, NH4H2PO4was added as a phosphorus source in the process of the hydrothermal treatment of melamine for the first time, and phosphorus-doped hollow tubular g-C3N4(x-P-HCN) was fabricated and used for photocatalytic CO2reduction. Here, 1.0-P-HCN exhibited the largest CO production rate of 9.00 μmol·g−1·h−1, which was 10.22 times higher than that of bulk g-C3N4. After doping with phosphorus, the light absorption range, the CO2adsorption capacity, and the specific surface area of the 1.0-P-HCN sample were greatly improved. In addition, the separation of photogenerated electron–hole pairs was enhanced. Furthermore, the phosphorus-doped g-C3N4effectively activated the CO2adsorbed on the surface of phosphorus-doped g-C3N4photocatalysts, which greatly enhanced the CO production rate of photocatalytic CO2reduction over that of g-C3N4.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 31
·期 5
·7027-7042
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IF 5.8
Chen Xuewen,Quan Hongping,Yu Jie,Hu Yuling,Huang Zhiyu
In order to reduce the impact of greenhouse gases on the environment, the development of various new CO 2 capture materials has become a hot spot. In this work, a novel composite amine solid adsorbent was prepared by simultaneously using tetraethylenepentamine (TEPA) and 2-[2-(dimethylamino) ethoxy] ethanol (DMAEE) for amine functionalization on the polyester microsphere carrier. The introduction of methyl methacrylate (MMA) with high glass transition temperature into the polyester carrier makes the carrier microspheres have high hardness. At the same time, the carrier also contains active epoxy groups and hydrophobic glycidyl methacrylate (GMA, which can undergo ring-opening reaction with composite amines to achieve high-load and low-energy chemical grafting of amines on the carrier. The composite aminated polyester microspheres were used as an efficient adsorbent for CO 2 in simulated flue gas. The results show that the synergistic effect of TEPA-DMAEE composite amine system in the adsorbent is beneficial to the improvement of CO 2 capture capacity. When the total amine content in the impregnating solution is 45 wt% and the composite amine ratio is TEPA: DMAEE = 6: 4, the CO 2 adsorption capacity can reach the optimal value of 2.45 mmol/ g at 70 °C. In addition, the composite amine microsphere adsorbent has cyclic regeneration performance. Importantly, through kinetic fitting, the Avrami kinetic model fits the CO 2 adsorption better than the quasi-first-order and quasi-second-order kinetic models, which proves that physical adsorption and chemical adsorption coexist in the adsorption process. This simple, long-term stable and excellent selective separation performance makes amine-functionalized adsorbents have potential application prospects in CO 2 capture. Graphical abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Yangguan Chen,Jinrui Zhang,Haorui Liu,Xiaoqiong Wang,Shuixia Chen
Solid-amine adsorbents are promising CO 2 post-combustion adsorption materials to mitigate global warming. As one of the most important evaluation criteria, the CO 2 adsorption capacity of the adsorbent was determined by both kinetic and thermodynamic factors, while high temperature is good for mass transfer and low temperature is advantageous for equilibrium to move towards adsorption. In this study, surfactants were added into polyethylenimine (PEI) cryogel to enhance mass transfer and reduce the adsorption temperature, thereby promoting its adsorption capacity. With the addition of polyethylene glycol (PEG200), the CO 2 adsorption capacity reached a maximum value of 6.48 mmol/g at 65 °C, and the amine efficiency reached a maximum value of 0.52 mol C/mol N at 45 °C. Further characterization revealed that the addition of PEG not only enhanced the mass transfer, but also changed the chemisorption mechanisms, which were very similar to the effects of water. Besides, PEG would form hydrogen bonds with the PEI polymer network and showed stable regeneration capacity, thereby exhibiting a greater application potential.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Zhu Jiexin,Li Jiantao,Lu Ruihu,Yu Ruohan,Zhao Shiyong,Li Chengbo,Lv Lei,Xia Lixue,Chen Xingbao,Cai Wenwei,Meng Jiashen,Zhang Wei,Pan Xuelei,Hong Xufeng,Dai Yuhang,Mao Yu,Li Jiong,Zhou Liang,He Guanjie,Pang Quanquan,Zhao Yan,Xia Chuan,Wang Ziyun,Dai Liming,Mai Liqiang
Electrochemical conversion of CO 2 to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a Bi 3 S 2 nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages. Specifically, a more than 95% faraday efficiency was achieved for the formate formation over a wide potential range above 1.0 V and at ampere-level current densities. The observed excellent catalytic performance was attributable to a unique reconstruction mechanism to form more defective sites while the ascorbic acid layer further stabilized the defective sites by trapping the poisoning hydroxyl groups. When used in an all-solid-state reactor system, the newly developed catalyst achieved efficient production of pure formic acid over 120 hours at 50 mA cm –2 (200 mA cell current).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chaopeng Zhang,Chenguang Li,Wenjie Li,Xin Guo
Li 4 SiO 4 shows great promise for cyclic high-temperature CO 2 capture due to its excellent stability, high capacity, and low regeneration temperature. However, the practical application of Li 4 SiO 4 is mainly limited by the high cost of raw materials, particularly lithium resources. Additionally, the heavy use of lithium-ion batteries (LIBs) in developing renewable energy sources raises concerns about the disposal of many waste LIBs. This article synthesized Li 4 SiO 4 sorbent (BR-Li 4 SiO 4 ) using spent lithium cobalt oxide (LiCoO 2 ) cathodes and rice husk ash for CO 2 capture. Meanwhile, we also prepared R-Li 4 SiO 4 /P-Li 4 SiO 4 using commercial Li 2 CO 3 and rice husk ash/commercial crystalline SiO 2 as a comparison. The results show that the BR-Li 4 SiO 4 sorbent exhibited excellent CO 2 capture capacity and cycling stability at 675 °C, maintaining a stable capacity of 0.28 g/g under 100% CO 2 after 30 cycles. BR-Li 4 SiO 4 also demonstrated significantly reduced costs and a superior microstructure compared to R-Li 4 SiO 4 and P-Li 4 SiO 4 . Furthermore, the impact of a simulated flue gas containing 15% CO 2 and 10% H 2 O on Li 4 SiO 4 adsorption was investigated. It was found that the adsorption of CO 2 was decreased at low CO 2 concentrations, but the addition of 10% H 2 O showed a slight enhancement in CO 2 adsorption. Under a mixture of 15% CO 2 + 10% H 2 O (balanced with N 2 ), the maximum adsorption capacity of BR-Li 4 SiO 4 was 0.17 g/g, and its optimal adsorption temperature decreased by 50 °C to 625 °C compared to 15% CO 2 . Therefore, this study will provide valuable insights into the industrial application of Li 4 SiO 4 in CO 2 adsorption.
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