| 1. |
- Liu, Yanrong, et al.
(författare)
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Ionic liquids/deep eutectic solvents for CO2 capture: Reviewing and evaluating
- 2021
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Ingår i: Green Energy & Environment. - : Elsevier. - 2468-0257. ; 6:3, s. 314-328
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Tidskriftsartikel (refereegranskat)abstract
- The CO2 solubilities (including CO2 Henry’s constant) in physical- and chemical-based ILs/DESs and the COSMO-RS models describing these properties were comprehensively collected and summarized. The summarized results indicate that chemical-based ILs/DESs are superior to physical-based ILs/DESs for CO2 capture, especially those ILs have functionalized cation and anion, and superbase DESs; some of the superbase DESs have higher CO2 solubilities than those of ILs; the best physical- and chemical-based ILs, as well as physical- and chemical-based DESs are [BMIM][BF4] (4.20 mol kg-1), [DETAH][Im] (11.91 mol kg-1), [L-Arg]-Gly 1:6 (4.92 mol kg-1) and TBD-EG 1:4 (12.90 mol kg-1), respectively. Besides the original COSMO-RS mainly providing qualitative predictions, six corrected COSMO-RS models have been proposed to improve the prediction performance based on the experimental data, but only one model is with universal parameters. The newly determined experimental results were further used to verify the perditions of original and corrected COSMO-RS models. The comparison indicates that the original COSMO-RS qualitatively predicts CO2 solubility for some but not all ILs/DESs, while the quantitative prediction is incapable at all. The original COSMO-RS is capable to predict CO2 Henry’s constant qualitatively for both physical-based ILs and DESs, and quantitative prediction is only available for DESs. For the corrected COSMO-RS models, only the model with universal parameters provides quantitative predictions for CO2 solubility in physical-based DESs, while other corrected models always show large deviations (>83%) compared with the experimental CO2 Henry’s constants.
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| 2. |
- Zhang, Zhibo, et al.
(författare)
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Encapsulation of multiple enzymes in a metal–organic framework with enhanced electro-enzymatic reduction of CO2 to methanol
- 2021
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Ingår i: Green Chemistry. - : Royal Society of Chemistry. - 1463-9262 .- 1463-9270. ; 23:6, s. 2362-2371
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Tidskriftsartikel (refereegranskat)abstract
- Efficient enzymatic conversion of CO2 to methanol is limited by low CO2 solubility in water (33 mM), and the high-cost of the cofactor (NADH) hinders the potential large-scale application of CO2 enzymatic conversion. In this study, a bioelectrocatalytic system was established for tackling both these issues, and in this system enzymes were embedded in the metal–organic framework ZIF-8 via in situ encapsulation to increase the substrate (CO2) concentration and pre-concentrate NADH, and a Rh complex-grafted electrode was developed for regenerating NADH in a sustainable manner. The results showed that after encapsulation of enzymes in ZIF-8, the methanol concentration increased from 0.061 to 0.320 mM (5 fold) in three hours. Furthermore, after coupling with electrocatalytic NADH regeneration, the methanol concentration further increased to 0.742 mM (12 fold) compared to a free enzyme system. Overall, methanol was produced at a rate of 822 μmol g−1 h−1.
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| 3. |
- Zhang, Zhibo, et al.
(författare)
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Zinc-based deep eutectic solvent – An efficient carbonic anhydrase mimic for CO2 hydration and conversion
- 2021
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Ingår i: Separation and Purification Technology. - : Elsevier. - 1383-5866 .- 1873-3794. ; 276
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Tidskriftsartikel (refereegranskat)abstract
- Carbonic anhydrase (CA) has demonstrated great potential to mitigate CO2 emissions by enzymatic conversion of CO2, while its commercial implementation is limited by the inherent shortcomings of CA, such as thermal and chemical instability, high sensitivity to the environment, and high cost. To overcome the drawbacks of CA and develop advanced technologies for mitigating CO2 emission, for the first time, mimetic CA (ZnHisGly) with the characteristics of natural CA was designed and synthesized, i.e., zinc-based deep eutectic solvent (DES), to boost CO2 hydration and conversion. The mimetic CA exhibited facile synthesis, high stability, and low cost as the characteristics of DES, and showed better catalytic performance compared to the currently reported mimetic CA. Particularly, its catalytic performance increased greatly with increasing pH and temperatures, which provides promising prospects in the industrial applications of DES-based CA mimics.
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| 4. |
- Xu, Weidong, 1988-, et al.
(författare)
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Rational molecular passivation for high-performance perovskite light-emitting diodes
- 2019
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Ingår i: Nature Photonics. - : Springer Nature Publishing AG. - 1749-4885 .- 1749-4893. ; 13:6, s. 418-424
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Tidskriftsartikel (refereegranskat)abstract
- A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecules has been identified as an attractive approach to tackle this issue. However, implementation of this approach has been hindered by a lack of deep understanding of how the molecular structures influence the effectiveness of passivation. We show that the so far largely ignored hydrogen bonds play a critical role in affecting the passivation. By weakening the hydrogen bonding between the passivating functional moieties and the organic cation featuring in the perovskite, we significantly enhance the interaction with defect sites and minimize non-radiative recombination losses. Consequently, we achieve exceptionally high-performance near-infrared perovskite light-emitting diodes with a record external quantum efficiency of 21.6%. In addition, our passivated perovskite light-emitting diodes maintain a high external quantum efficiency of 20.1% and a wall-plug efficiency of 11.0% at a high current density of 200 mA cm−2, making them more attractive than the most efficient organic and quantum-dot light-emitting diodes at high excitations.
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| 5. |
- Zhang, Zhibo, et al.
(författare)
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Application and Challenge of Ionic Liquids as Co-solvent for Electro-enzymatic Conversion of CO2 to Methanol
- 2021
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Ingår i: Proceedings of the Chinese Society of Electrical Engineering. - : Chinese Society for Electrical Engineering. - 0258-8013. ; 41:11, s. 3657-3665
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Tidskriftsartikel (refereegranskat)abstract
- Utilization of carbon dioxide (CO2) has attracted great research interests, because CO2 is both a typical greenhouse gas and renewable carbon resource. This review mainly summarized and reviewed the research work linked to the challenges in the enzymatic conversion of CO2, such as NADH regeneration and low CO2 conversion efficiency. Based on the summary on the electro-enzymatic conversion of CO2, ionic liquids for the enzymatic conversion of CO2, and ionic liquids for the electrochemical conversion of CO2, we suggested applying ionic liquids as co-solvent in the enzymatic conversion of CO2 to methanol and coupling it with the reduction of NAD+ to NADH by electrocatalysis, providing a novel pathway for producing methanol from CO2.
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| 6. |
- Zhang, Zhibo, et al.
(författare)
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Developing and Regenerating Cofactors for Sustainable Enzymatic CO2 Conversion
- 2022
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Ingår i: Processes. - : MDPI. - 2227-9717. ; 10:2
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Tidskriftsartikel (refereegranskat)abstract
- Enzymatic CO2 conversion offers a promising strategy for alleviating global warming and promoting renewable energy exploitation, while the high cost of cofactors is a bottleneck for large-scale applications. To address the challenge, cofactor regeneration is usually coupled with the enzymatic reaction. Meanwhile, artificial cofactors have been developed to further improve conversion efficiency and decrease cost. In this review, the methods, such as enzymatic, chemical, electrochemical, and photochemical catalysis, developed for cofactor regeneration, together with those developed artificial cofactors, were summarized and compared to offer a solution for large-scale enzymatic CO2 conversion in a sustainable way.
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| 7. |
- Zhang, Zhibo, et al.
(författare)
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Natural Deep Eutectic Solvents Enhanced Electro-Enzymatic Conversion of CO2 to Methanol
- 2022
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Ingår i: Frontiers in Chemistry. - : Frontiers Media S.A.. - 2296-2646. ; 10
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Tidskriftsartikel (refereegranskat)abstract
- Electro-enzymatic conversion of CO2 offers a promising solution for CO2 utilization, while the conversion rate and efficiency were disappointing. To address the challenge, four kinds of natural deep eutectic solvents (NADES) with desirable biocompatibility were developed for the first time and used as the co-electrolyte in the electro-enzymatic conversion of CO2. As a result, the SerGly-based solution presents high CO2 solubility and high electrocatalytic activity, compared to the conventional buffer. By applying SerGly in the electro-enzymatic conversion of CO2, the yield of the product (methanol) is two times higher than that in the Tris-HCl buffer (0.22 mM) and 16 times higher than the control reaction.
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| 8. |
- Zhang, Zhibo, et al.
(författare)
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Novel artificial ionic cofactors for efficient electro-enzymatic conversion of CO2 to formic acid
- 2022
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Ingår i: Journal of CO2 Utilization. - : Elsevier. - 2212-9820 .- 2212-9839. ; 60
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Tidskriftsartikel (refereegranskat)abstract
- The low yield of enzymatic conversion of CO2 to formic acid as well as the high cost and instability of using the natural cofactor (NADH) hamper the large-scale application of the CO2 enzymatic utilization. To address these issues and to improve the production of formic acid, six bipyridinium-based artificial cofactors were developed for the enzymatic conversion of CO2 and further integrated with the electrocatalytic regeneration of the cofactors for the formic acid production. All of them did show a higher catalytic performance compared to NADH. Particularly, 1,1′-bis(2-(dimethylamino)ethyl)-4,4′-bipyridinium bromine did exhibit the highest catalytic performance with a high formic acid concentration of 4.76 mM in 60 min, which is 47 times higher than that of the natural cofactor NADH and is also currently the highest performance among the reported artificial cofactors in literature. Thermodynamic analysis, electrochemical investigations, and molecular dynamics simulations were performed to clarify the structure-energy relationship of the functional bipyridinium-based salts and to rationalize how it is affected by the different functional groups. This study gives a deep insight into the role of artificial cofactors in enzymatic reactions and can clearly promote the development of novel bioelectrochemical conversion of CO2.
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| 9. |
- Bao, Chunxiong, et al.
(författare)
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High Performance and Stable All-Inorganic Metal Halide Perovskite-Based Photodetectors for Optical Communication Applications
- 2018
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Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 30:38
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Tidskriftsartikel (refereegranskat)abstract
- Photodetectors are critical parts of an optical communication system for achieving efficient photoelectronic conversion of signals, and the response speed directly determines the bandwidth of the whole system. Metal halide perovskites, an emerging class of low-cost solution-processed semiconductors, exhibiting strong optical absorption, low trap states, and high carrier mobility, are widely investigated in photodetection applications. Herein, through optimizing the device engineering and film quality, high-performance photodetectors based on all-inorganic cesium lead halide perovskite (CsPbIxBr3-x), which simultaneously possess high sensitivity and fast response, are demonstrated. The optimized devices processed from CsPbIBr2 perovskite show a practically measured detectable limit of about 21.5 pW cm(-2) and a fast response time of 20 ns, which are both among the highest reported device performance of perovskite-based photodetectors. Moreover, the photodetectors exhibit outstanding long-term environmental stability, with negligible degradation of the photoresponse property after 2000 h under ambient conditions. In addition, the resulting perovskite photodetector is successfully integrated into an optical communication system and its applications as an optical signal receiver on transmitting text and audio signals is demonstrated. The results suggest that all-inorganic metal halide perovskite-based photodetectors have great application potential for optical communication.
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| 10. |
- Duan, Dongban, et al.
(författare)
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Gadolinium Neutron Capture Reaction-Induced Nucleodynamic Therapy Potentiates Antitumor Immunity
- 2023
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Ingår i: CCS Chemistry. - : Chinese Chemical Society. - 2096-5745. ; 5:11, s. 2589-2602
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Tidskriftsartikel (refereegranskat)abstract
- A nuclear reaction-induced dynamic therapy, denoted as nucleodynamic therapy (NDT), has been invented that triggers immunogenic cell death and successfully treats metastatic tumors due to its unexpected abscopal effect. Gadolinium neutron capture therapy (GdNCT) is binary radiotherapy based on a localized nuclear reaction that produces high-energy radiations (e.g., Auger electrons, γ-rays, etc.) in cancer cells when 157Gd is irradiated with thermal neutrons. Yet, its clinical application has been postponed due to the poor ability of Auger electrons and γ-rays to kill cells. Here, we engineered a 157Gd-porphyrin framework that synergizes GdNCT and dynamic therapy to efficiently produce both •OH and immunogenic 1O2 in cancer cells, thereby provoking a strong antitumor immune response. This study unveils the fact and mechanism that NDT heats tumor immunity. Another unexpected finding is that the Auger electron can be the most effective energy-transfer medium for radiation-induced activation of nanomedicines because its nanoscale trajectory perfectly matches the size of nanomaterials. In mouse tumor models, NDT causes nearly complete regression of both primary and distant tumor grafts. Thus, this 157Gd-porphyrin framework radioenhancer endows GdNCT with the exotic function of triggering dynamic therapy; its application may expand in clinics as a new radiotherapy modality that utilizes GdNCT to provoke whole-body antitumor immune response for treating metastases, which are responsible for 90% of all cancer deaths.
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