期刊:Nature
作者:Junliang Sun, Charlotte Bonneau, Ángel Cantín, Avelino Corma, María J. Díaz-Cabañas, Manuel Moliner, Daliang Zhang, Mingrun Li & Xiaodong Zou*
时间:2009年4月30日
Nature, volume 458, pages 1154–1157 (2009)
Nature, volume 524, pages 74–78 (2015)
Nature Chemistry, volume 12, pages 620–628 (2020)
Cell, volume 148, issues 1–2, pages 213-227
期刊:Nature
作者:Peng Guo, Jiho Shin, Alex G. Greenaway, Jung Gi Min, Jie Su, Hyun June Choi, Leifeng Liu, Paul A. Cox, Suk Bong Hong, Paul A. Wright and Xiaodong Zou*
时间:2015年7月15日
期刊:Nature
作者:Lei Gao, Cong Su, Xiaoxia Du, Ruishan Wang, Shuming Chen, Yu Zhou, Chengwei Liu, Xiaojing Liu, Runze Tian, Liyun Zhang, Kebo Xie, She Chen, Qianqian Guo, Lanping Guo, Yoshio Hano, Manabu Shimazaki, Atsushi Minami, Hideaki Oikawa, Niu Huang, K. N. Houk, Luqi Huang, Jungui Dai and Xiaoguang Lei*
时间:2020年5月25日
期刊:Cell
作者:LimingSun, HuayiWang, ZhigaoWang, SudanHe, SheChen, DaohongLiao, LaiWang, JiacongYan, WeilongLiu, XiaoguangLei, XiaodongWang
时间:2012年1月20日
The prediction and synthesis of new crystal structures enable the targeted preparation of materials with desired properties. Among porous solids, this has been achieved for metal–organic frameworks1,2,3, but not for the more widely applicable zeolites4,5, where new materials are usually discovered using exploratory synthesis. Although millions of hypothetical zeolite structures have been proposed6,7, not enough is known about their synthesis mechanism to allow any given structure to be prepared. Here we present an approach that combines structure solution with structure prediction, and inspires the targeted synthesis of new super-complex zeolites. We used electron diffraction to identify a family of related structures and to discover the structural ‘coding’ within them. This allowed us to determine the complex, and previously unknown, structure of zeolite ZSM-25 (ref. 8), which has the largest unit-cell volume of all known zeolites (91,554 cubic ångströms) and demonstrates selective CO2 adsorption. By extending our method, we were able to predict other members of a family of increasingly complex, but structurally related, zeolites and to synthesize two more-complex zeolites in the family, PST-20 and PST-25, with much larger cell volumes (166,988 and 275,178 cubic ångströms, respectively) and similar selective adsorption properties. Members of this family have the same symmetry, but an expanding unit cell, and are related by hitherto unrecognized structural principles; we call these family members embedded isoreticular zeolite structures.
The synthesis of crystalline molecular sieves with pore dimensions that fill the gap between microporous and mesoporous materials is a matter of fundamental and industrial interest(1-3). The preparation of zeolitic materials with extralarge pores and chiral frameworks would permit many new applications. Two important steps in this direction include the synthesis(4) of ITQ-33, a stable zeolite with 18 x 10 x 10 ring windows, and the synthesis(5) of SU-32, which has an intrinsically chiral zeolite structure and where each crystal exhibits only one handedness. Here we present a germanosilicate zeolite (ITQ-37) with extralarge 30-ring windows. Its structure was determined by combining selected area electron diffraction ( SAED) and powder X-ray diffraction (PXRD) in a charge-flipping algorithm(6). The framework follows the SrSi2 (srs) minimal net(7) and forms two unique cavities, each of which is connected to three other cavities to form a gyroidal channel system. These cavities comprise the enantiomorphous srs net of the framework. ITQ-37  is the first chiral zeolite with one single gyroidal channel. It has the lowest framework density (10.3 T atoms per 1,000 angstrom(3)) of all existing 4-coordinated crystalline oxide frameworks, and the pore volume of the corresponding silica polymorph would be 0.38 cm(3) g(-1).
The Diels–Alder reaction is one of the most powerful and widely used methods in synthetic chemistry for the stereospecific construction of carbon–carbon bonds. Despite the importance of Diels–Alder reactions in the biosynthesis of numerous secondary metabolites, no naturally occurring stand-alone Diels–Alderase has been demonstrated to catalyse intermolecular Diels–Alder transformations. Here we report a flavin adenine dinucleotide-dependent enzyme, Morus alba Diels–Alderase (MaDA), from Morus cell cultures, that catalyses an intermolecular [4+2] cycloaddition to produce the natural isoprenylated flavonoid chalcomoracin with a high efficiency and enantioselectivity. Density functional theory calculations and preliminary measurements of the kinetic isotope effects establish a concerted but asynchronous pericyclic pathway. Structure-guided mutagenesis and docking studies demonstrate the interactions of MaDA with the diene and dienophile to catalyse the [4+2] cycloaddition. MaDA exhibits a substrate promiscuity towards both dienes and dienophiles, which enables the expedient syntheses of structurally diverse natural products. We also report a biosynthetic intermediate probe (BIP)-based target identification strategy used to discover MaDA.
The receptor-interacting serine-threonine kinase 3 (RIP3) is a key signaling molecule in the programmed necrosis (necroptosis) pathway. This pathway plays important roles in a variety of physiological and pathological conditions, including development, tissue damage response, and antiviral immunity. Here, we report the identification of a small molecule called (E)-N-(4-(N-(3-methoxypyrazin-2-yl)sulfamoyl)phenyl)-3-(5-nitrothiophene-2-yl)acrylamidehereafter referred to as necrosulfonamidethat specifically blocks necrosis downstream of RIP3 activation. An affinity probe derived from necrosulfonamide and coimmunoprecipitation using anti-RIP3 antibodies both identified the mixed lineage kinase domain-like protein (MLKL) as the interacting target. MLKL was phosphorylated by RIP3 at the threonine 357 and serine 358 residues, and these phosphorylation events were critical for necrosis. Treating cells with necrosulfonamide or knocking down MLKL expression arrested necrosis at a specific step at which RIP3 formed discrete punctae in cells. These findings implicate MLKL as a key mediator of necrosis signaling downstream of the kinase RIP3.