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91.
以某低渗透油藏为对象,首先在数据挖掘的基础上制定了低渗透油藏注CO_2驱筛选标准.基于模糊综合评价法,建立了适用于低渗透油藏CO_2驱适宜度评价的模糊综合评价模型,并运用该模型对目标油藏注CO_2的适宜度进行了评价.计算结果表明目标油藏注气驱开发适应性较好.评价过程有效地降低了直接进行注气开发的风险,为之后低渗透油藏注气开发提供了技术和经济上的指导. 相似文献
92.
Virasoro constraint is the operator algebra version of one-loop equation for a Hermitian one-matrix model, and it plays an important role in solving the model. We construct the realization of the Virasoro constraint from the Conformal Field Theory (CFT) method. From multi-loop equations of the one-matrix model, we get a more general constraint. It can be expressed in terms of the operator algebras, which is the Virasoro subalgebra with extra parameters. In this sense, we named as generalized Virasoro constraint. We enlarge this algebra with central extension, this is a new kind of algebra, and the usual Virasoro algebra is its subalgebra. And we give a bosonic realization of its subalgebra. 相似文献
93.
Shaopeng Li Jing Du Bin Zhang Yanzhen Liu Qingqing Mei Qinglei Meng Minghua Dong Juan Du Zhijuan Zhao Lirong Zheng Buxing Han Meiting Zhao Huizhen Liu 《物理化学学报》2023,38(10):2206019
Selective hydrogenation is a vital class of reaction. Various unsaturated functional groups in organic compounds, such as aromatic rings, alkynyl (C≡C), carbonyl (C=O), nitro (-NO2), and alkenyl (C=C) groups, are typical targets in selective hydrogenation. Therefore, selectivity is a key indicator of the efficiency of a designed hydrogenation reaction. 5-(Hydroxymethyl)furfural (HMF) is an important platform compound in the context of biomass conversion, and recently, the hydrogenation of HMF to produce fuels and other valuable chemicals has received significant attention. Controlling the selectivity of HMF hydrogenation is paramount because of the different reducible functional groups (C=O, C-OH, and C=C) in HMF. Moreover, the exploration of new routes for hydrogenating HMF to valuable chemicals is becoming attractive. 5-Methylfurfural (MF) is also an important organic compound; thus, the selective hydrogenation of HMF to MF is an essential synthetic route. However, this reaction has challenging thermodynamic and kinetic aspects, making it difficult to realize. Herein, we propose a strategy to design a highly efficient catalytic system for selective hydrogenation by exploiting the synergy between steric hindrance and hydrogen spillover. The design and preparation of the Pt@PVP/Nb2O5 catalyst (PVP = polyvinyl pyrrolidone; Nb2O5 = niobium(V) oxide) were also conducted. Surprisingly, HMF could be converted to MF with 92% selectivity at 100% HMF conversion. The reaction pathway was revealed through the combination of control experiments and density functional theory calculations. Although PVP blocked HMF from accessing the surface of Pt, hydrogen (H2) could be activated on the surface of Pt due to its small molecular size, and the activated H2 could migrate to the surface of Nb2O5 through a phenomenon called H2 spillover. The Lewis acidic surface of Nb2O5 could not adsorb the C=O group but could adsorb and activate the C-OH group of HMF; therefore, when HMF was adsorbed on Nb2O5, the C-OH groups were hydrogenated by the spilled over H2 to form MF. The high selectivity of this reaction was realized because of the unique combination of steric effects, hydrogen spillover, and tuning of the electronic states of the Pt and Nb2O5 surfaces. This new route for producing MF has great potential for practical application owing to its discovered advantages. We believe that this novel strategy can be used to design catalysts for other selective hydrogenation reactions. Furthermore, this study demonstrates a significant breakthrough in selective hydrogenation, which will be of interest to researchers working on the utilization of biomass, organic synthesis, catalysis, and other related fields.
相似文献
94.
多核过渡金属配合物作为一类广泛应用的均相催化剂,其设计灵感往往来自天然酶的多金属活性位点所发挥的重要作用.目前,三核金属配合物作为活化小分子的多金属催化剂受到了广泛的关注.为深入理解三核过渡金属配合物在催化反应中作用特点,对近年报道的代表性三核过渡金属配合物按金属中心进行分类,并对配体环境形成特点及催化应用进行综述.从金属中心出发,讨论了三核过渡金属配合物的几何结构和电子特征;从配体环境出发,总结了关联三个独立的金属位点的配位环境特征;在催化应用方面,重点综述了三核过渡金属配合物在涉及特定化学键活化反应的催化作用机制,最后对三核过渡金属配合物的催化应用前景进行展望. 相似文献
95.
Dr. Liping Liu Dr. Haibing Meng Dr. Yongqiang Chai Dr. Xianjie Chen Dr. Jingyi Xu Dr. Xiaolong Liu Dr. Weixu Liu Prof. Dirk M. Guldi Prof. Yongfa Zhu 《Angewandte Chemie (International ed. in English)》2023,62(11):e202217897
High-efficiency photocatalysts based on metal-organic frameworks (MOFs) are often limited by poor charge separation and slow charge-transfer kinetics. Herein, a novel MOF photocatalyst is successfully constructed by encapsulating C60 into a nano-sized zirconium-based MOF, NU-901. By virtue of host-guest interactions and uneven charge distribution, a substantial electrostatic potential difference is set-up in C60@NU-901. The direct consequence is a robust built-in electric field, which tends to be 10.7 times higher in C60@NU-901 than that found in NU-901. In the catalyst, photogenerated charge carriers are efficiently separated and transported to the surface. For example, photocatalytic hydrogen evolution reaches 22.3 mmol g−1 h−1 for C60@NU-901, which is among the highest values for MOFs. Our concept of enhancing charge separation by harnessing host-guest interactions constitutes a promising strategy to design photocatalysts for efficient solar-to-chemical energy conversion. 相似文献
96.
Helian Li Yongxin Zhang Xiaoxiao Yang Zhenxi Deng Zhimin Zhu Pan Zhou Xinke Ouyang Yuting Yuan Xi Chen Lingyue Yang Meng Liu Prof. Dr. Chao Shu 《Angewandte Chemie (International ed. in English)》2023,62(15):e202300159
Despite the significance of sultines in synthesis, medicine, and materials science, the chemistry of sultines has remained unexplored due to their inaccessibility. Herein, we demonstrate the development of a photoredox-catalyzed multifluoromethyl radical addition/SO2 incorporation/polar cyclization cascade approach to multifluoromethylated γ-sultines. The reactions proceed by single electron transfer induced multifluoromethyl radical addition to an alkene followed by SO2 incorporation, and single-electron reduction for polar 5-exo-tet cyclization. Key to the success of the protocol is the use of easily oxidizable multifluoroalkanesulfinates as bifunctional reagents. The reactions proceed with excellent functional-group tolerance to deliver γ-sultines in moderate to excellent yields. 相似文献
97.
Dr. Rongli Mi Dr. Lingzhen Zeng Maolin Wang Shuheng Tian Jie Yan Shixiang Yu Dr. Meng Wang Prof. Ding Ma 《Angewandte Chemie (International ed. in English)》2023,62(28):e202304219
The utilization of carbon resources stored in plastic polymers through chemical recycling and upcycling is a promising approach for mitigating plastic waste. However, most current methods for upcycling suffer from limited selectivity towards a specific valuable product, particularly when attempting full conversion of the plastic. We present a highly selective reaction route for transforming polylactic acid (PLA) into 1,2-propanediol utilizing a Zn-modified Cu catalyst. This reaction exhibits excellent reactivity (0.65 g gcat−1 h−1) and selectivity (99.5 %) towards 1,2-propanediol, and most importantly, can be performed in a solvent-free mode. Significantly, the overall solvent-free reaction is an atom-economical reaction with all the atoms in reactants (PLA and H2) fixed into the final product (1,2-propanediol), eliminating the need for a separation process. This method provides an innovative and economically viable solution for upgrading polyesters to produce high-purity products under mild conditions with optimal atom utilization. 相似文献
98.
Bing Qin Zhi-Long Yu Jin Huang Yu-Feng Meng Rui Chen Zhi Chen Shu-Hong Yu 《Angewandte Chemie (International ed. in English)》2023,62(5):e202214809
Cellulose aerogels are plagued by intermolecular hydrogen bond-induced structural plasticity, otherwise rely on chemicals modification to extend service life. Here, we demonstrate a petrochemical-free strategy to fabricate superelastic cellulose aerogels by designing hierarchical structures at multi scales. Oriented channels consolidate the whole architecture. Porous walls of dehydrated cellulose derived from thermal etching not only exhibit decreased rigidity and stickiness, but also guide the microscopic deformation and mitigate localized large strain, preventing structural collapse. The aerogels show exceptional stability, including temperature-invariant elasticity, fatigue resistance (∼5 % plastic deformation after 105 cycles), high angular recovery speed (1475.4° s−1), outperforming most cellulose-based aerogels. This benign strategy retains the biosafety of biomass and provides an alternative filter material for health-related applications, such as face masks and air purification. 相似文献
99.
Dr. Meng Lu Shuai-Bing Zhang Ming-Yi Yang Yu-Fei Liu Jia-Peng Liao Pei Huang Dr. Mi Zhang Prof. Shun-Li Li Prof. Zhong-Min Su Prof. Ya-Qian Lan 《Angewandte Chemie (International ed. in English)》2023,62(31):e202307632
In this work, we innovatively assembled two types of traditional photosensitizers, that is pyridine ruthenium/ferrum (Ru(bpy)32+/Fe(bpy)32+) and porphyrin/metalloporphyrin complex (2HPor/ZnPor) by covalent linkage to get a series of dual photosensitizer-based three-dimensional metal-covalent organic frameworks (3D MCOFs), which behaved strong visible light-absorbing ability, efficient electron transfer and suitable band gap for highly efficient photocatalytic hydrogen (H2) evolution. Rubpy-ZnPor COF achieved the highest H2 yield (30 338 μmol g−1 h−1) with apparent quantum efficiency (AQE) of 9.68 %@420 nm, which showed one of the best performances among all reported COF based photocatalysts. Furthermore, the in situ produced H2 was successfully tandem used in the alkyne hydrogenation with ≈99.9 % conversion efficiency. Theoretical calculations reveal that both the two photosensitizer units in MCOFs can be photoexcited and thus contribute optimal photocatalytic activity. This work develops a general strategy and shows the great potential of using multiple photosensitive materials in the field of photocatalysis. 相似文献
100.
Ning Ling Jiguang Zhang Meng Wang Zhen Wang Ziyu Mi Surani Bin Dolmanan Mingsheng Zhang Bingqing Wang Wan Ru Leow Jia Zhang Yanwei Lum 《Angewandte Chemie (International ed. in English)》2023,62(36):e202308782
Electrochemical CO2 reduction (CO2R) in acidic media with Cu-based catalysts tends to suffer from lowered selectivity towards multicarbon products. This could in principle be mitigated using tandem catalysis, whereby the *CO coverage on Cu is increased by introducing a CO generating catalyst (e.g. Ag) in close proximity. Although this has seen significant success in neutral/alkaline media, here we report that such a strategy becomes impeded in acidic electrolyte. This was investigated through the co-reduction of 13CO2/12CO mixtures using a series of Cu and CuAg catalysts. These experiments provide strong evidence for the occurrence of tandem catalysis in neutral media and its curtailment under acidic conditions. Density functional theory simulations suggest that the presence of H3O+ weakens the *CO binding energy of Cu, preventing effective utilization of tandem-supplied CO. Our findings also provide other unanticipated insights into the tandem catalysis reaction pathway and important design considerations for effective CO2R in acidic media. 相似文献