中国化学印记

中国化学印记

2017 年《化学进展》在新一届编委会的策划下，特别设立 “ 中国化学印记 ” 栏目，该栏目旨在述评中国化学研究者在国际顶级学术期刊 Nature 和 Science 等上刊发的原创性工作，每年出版一次，刊登在次年的第一期中。“中国化学印记”栏目的初衷是记录中国化学研究者在国际顶级期刊中留下的印记，将其载入史册，希望该栏目和《化学进展》的 Highlights 栏目一起成为记录我国化学工作者在国际化学研究界的里程碑式研究成果的一个窗口。2017 年“中国化学印记”栏目策划出版了 8 篇文章，这些文章的述评对象均为 2016 年中国化学学者以第一著作单位在 Nature 和 Science 上发表的论文，对其科学意义、研究背景、创新价值和社会影响进行述评。需要指出的是有一些论文已在国内其他化学期刊中有类似的述评文章发表，我们在此不再重复进行述评，但将其列出，供化学同行参考和交流。

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高容量富锂锰基正极材料的结构与电压衰减的起源与解决方案

尹祖伟, 孙世刚

2022, 34 (6): 1249-1251 | DOI: 10.7536/PC220624

录用日期: 2022-06-23

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摘要

Oxygen loss is the current mainstream explanation for voltage decay of Li-rich Mn-rich oxide cathode (LMR), which is conflictive with the ineffectiveness of trivial to stabilize its lattice oxygen and voltage decay. The unclear voltage decay mechanism of high-capacity Li-rich cathode hinders its commercial applications. In this finding, the driving force of voltage decay in LMR is attributed to its lattice displacement/strain, which is concluded by state-of-the-art multiscale characterizations and theoretical calculations, and harmonizes many aspects in this field. Dispersing the Li@Mn₆ units in layered structure is an effective method to stabilize the structure of LMR.

富勒烯“电子缓冲”机制与催化

王春儒, 李亚栋

2022, 34 (5): 1011-1012 | DOI: 10.7536/PC220435

录用日期: 2022-04-26

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摘要

Ethylene glycol was synthesized from dimethyl oxalate hydrogenation at ambient pressure over fullerene modified copper catalyst. Fullerenes show electron buffering effect to stabilize cuprous species and boost the copper catalysis. This finding provides a novel strategy for the design of stable catalysts using fullerenes as a molecular promoter.

沸石整体结构的刚性与局部孔道的柔性

肖丰收

2022, 34 (5): 1013-1014 | DOI: 10.7536/PC220508

录用日期: 2022-05-07

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摘要

Using in situ electron microscopy, it was directly observed that subcell flexibility of the zeolite framework occurred when benzene as a guest molecule was adsorbed into the straight channels of ZSM-5 zeolite nanosheets, where the opening pores stretched along the longest direction of confined benzene molecules with a maximum aspect change of 15%. This flexibility originates mainly from the topologically soft silicon-oxygen-silicon hinges between rigid tetrahedral SiO₄ units, which is very important for understanding molecular adsorption and shape selective catalysis.

面向产业化的全钙钛矿叠层光伏组件

孟磊, 李永舫

2022, 34 (6): 1247-1248 | DOI: 10.7536/PC220621

录用日期: 2022-06-23

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摘要

Hairen Tan's research group reported all-perovskite tandem solar modules achieving a certified PCE of 21.7% with an aperture area over 20 cm² and the device shows prominent ambient sta-bility, which demonstrates great potential for the perovskite solar cells toward commercialization.

高效合成热力学不稳定的双取代环己烷

董顺喜, 刘小华

2022, 34 (6): 1245-1246 | DOI: 10.7536/PC220527

录用日期: 2022-05-20

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摘要

Thermodynamically disfavored disubstituted cyclohexanes are synthesized with excellent kinetic stereocontrol from readily available substituted methylenecyclohexanes based on chain-walking catalysis. Control experiments and theoretical calculations suggest that the initial introduction of bulky boron ester substitution away from the ring is crucial to the high diastereoselectivity. This finding opens a new adventure to the application of chain walking catalysis in organic synthesis and provides a ready access to thermodynamically disfavored but biologically important disubstituted cyclohexanes and the derivatives.

原位制备过氧化氢实现尼龙单体的绿色合成

彭卿, 李亚栋

2022, 34 (5): 1015-1016 | DOI: 10.7536/PC220510

录用日期: 2022-05-07

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摘要

By using supported gold-palladium alloyed nanoparticles in conjunction with a titanium silicate-1 (TS-1) catalyst, H₂O₂ can be generated in situ as needed, producing cyclohexanone oxime with >95% selectivity, comparable to the current industrial route. The ammoximation of several additional simple ketones is also demonstrated. Our approach eliminates the need to transport and store highly concentrated, stabilized H₂O₂, potentially achieving substantial environmental and economic savings. This approach could form the basis of an alternative route to numerous chemical transformations that are currently dependent on a combination of preformed H₂O₂ and TS-1, while allowing for considerable process intensification.

手性纳米材料的免疫佐剂效应

曲广波, 江桂斌

2022, 34 (2): 239-240 | DOI: 10.7536/PC220220

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摘要

The chirality of nanoparticles determines their interaction with immune cells and the corre-spondent response in immune system. This finding provides a novel strategy for the design of vaccines to fight the infection of virus.

新型高效甲醇水相低温制氢催化剂

吴凯*

2017, 29 (8): 809-810 | DOI: 10.7536/PC170623

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摘要

Hydrogen stored in a chemical form as liquid organic compounds and released in-situ on demand through efficient catalytic processes at low temperature is a highly desirable hydrogen storage and transportation strategy. A recent breakthrough was reported by the Ma group at Peking University and their collaborators. They have developed a novel Pt/α-MoC catalyst with atomically dispersed Pt over α-MoC. The exceptional hydrogen production activity comes from the outstanding ability of α-MoC for water dissociation and the unique synergy between Pt and α-MoC for methanol activation and successive reforming processes.

反转吸附选择性可助金属有机框架纯化烯烃

陈邦林*

2017, 29 (8): 811-813 | DOI: 10.7536/PC170635

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摘要

Judicious utilization of host-guest supramolecular interactions and flexibilities of both the host and guest enables metal-organic frameworks to show abnormal adsorption selectivities for the less polar, more saturated hydrocarbons, which is useful for efficient purification of high-value alkenes such as ethylene and butadiene.

被引次数 :

( 1 )

对称性匹配调控水平单壁碳纳米管阵列手性

朱振兴, 魏飞

2017, 29 (6): 579-581 | DOI: 10.7536/PC170528

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摘要

Controllable synthesis of horizontally aligned single walled carbon nanotubes (SWNTs) with specific chirality and high areal density remains a challenge.A recent breakthrough was achieved by the Jin Zhang's group from Peking University.They proposed a feasible route towards tuning the chirality of epitaxially-grown aligned SWNTs according to the designed catalyst lattice symmetry.With different uniform metal carbide catalysts,two different types of aligned SWNTs with specific structures, the metallic (12,6) and semiconducting (8,4) ones,can be synthesized separately with their chiral selectivity both over 80%,tandem with a high density of more than 10 tubes/μm.These exciting results clearly demonstrate that it is possible to control SWNTs'structures based on the symmetry matching in structures between SWNTs and crystal surface of catalyst particles.

中国化学印记介绍

2017, 29 (1): 0-0 |

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摘要

类细胞环境下蛋白质结构与功能的NMR研究

徐国华, 李从刚, 刘买利

2017, 29 (1): 75-82 | DOI: 10.7536/PC161225

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摘要

细胞环境是大多数蛋白质行使其功能的天然环境。在细胞环境中，大分子拥挤、限域、弱相互作用等普遍存在，已经有越来越多的研究表明这种复杂细胞环境会影响蛋白质的结构与功能。因此，在越接近天然的环境中研究蛋白质，越有可能揭示蛋白质功能的本质。蛋白质结构与功能的原位研究已是目前蛋白质科学中的前沿领域。核磁共振波谱技术是研究复杂环境中蛋白质结构与功能最具潜力的手段，它能提供原子分辨的蛋白质结构，动态与相互作用信息。本文总结了我们近几年利用核磁共振技术研究大分子拥挤、限域、以及原核E.coli细胞、非洲爪蟾卵母细胞中蛋白质结构与功能等方面取得的重要进展。

被引次数 :

( 1 )

超薄材料实现二氧化碳高效电催化还原

王潇乾, 吴宇恩, 李亚栋

2017, 29 (1): 1-2 | DOI: 10.7536/PC161235

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摘要

In a team of researchers at University of Science and Technology of China, partially oxidized atomic cobalt layers have been synthesized successfully and used to achieve efficient and robust CO₂ elecrtoreduction to formate. Such a new process may provide a path to convert CO₂ into useful fuels and thus help to alleviate energy crisis and global warming.

被引次数 :

( 1 )

猪笼草口缘超湿滑的揭密:Jiang-Taylor毛细升与液体定向输运

王树涛

2017, 29 (1): 3-4 | DOI: 10.7536/PC161236

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摘要

Unidirectional liquid spreading without energy input has plenty of promising applications such as bio-fluidics devices, bio-medical devices and self-lubrication. The secret of the fast continuous directional liquid transport on the peristome surface of Nepenthes alata was revealed-Jiang-Taylor capillary rise. This study will give new insights into the design of two-dimensional directional liquid transport.

晶面调控实现合成气低温制备烯烃过程

马丁

2017, 29 (1): 5-6 | DOI: 10.7536/PC161237

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摘要

Lower olefins are essential feedstock in polymeric industry, and therefore a direct syngas conversion route is challenging, yet highly demanding. Sun's group achieve 61% selectivity toward lower olefins over CoMn catalyst at mild conditions. It is found that the formation of Co₂C nanoprism with unique facets contributed to the astonishing performance.

铜催化的惰性苄位碳氢键的不对称氰基化反应

丁奎岭

2017, 29 (1): 13-14 | DOI: 10.7536/PC161238

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摘要

C-H bond functionalization refers to transformations that introduce functional group directly via the cleavage of C-H bond, which shows excellent step- and atom-economy. A recent breakthrough was achieved by the Guosheng Liu group in collaboration with Shannon S. Stahl group from University of Wisconsin-Madison. They discovered a new strategy to achieve Cu-catalyzed enantioselective cyanation of benzylic C-H bonds via a "Radical Relay Process". The present copper-catalyzed method provides a remarkably chemo-, regio- and enantioselectivity to afford optical organonitriles efficiently under mild reaction conditions.

离子杂化多孔材料分离乙炔和乙烯

张国俊, 孙宏伟

2017, 29 (1): 11-12 | DOI: 10.7536/PC161239

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摘要

The trade-off between adsorption capacity and selectivity of porous materials has been identified as a major challenge towards efficient gas separation/purification through physisorption. The research from Cui et al. address this daunting challenge by developing a new strategy that control over pore chemistry and pore size in hybrid porous materials enables the exploitation of supramolecular chemistry of gases to achieve both high capacity and selectivity, and sets new benchmarks for acetylene separation from ethylene.

碳酸钙变珍珠

姚沙沙, 刘昭明, 唐睿康

2017, 29 (1): 15-16 | DOI: 10.7536/PC161240

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摘要

A "assembly-and-mineralization" method is developed by Shuhong Yu's group from University of Science and Technology of China. It can fabricate nacre-like materials quickly at large scale by using controllable calcium carbonate mineralization, which is a great step to design and construct advanced functional materials by bioinspired approach.

被引次数 :

( 1 )

分子电子学重大突破:室温可逆稳定单分子器件

张小涛, 董焕丽, 胡文平

2017, 29 (1): 9-10 | DOI: 10.7536/PC170102

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摘要

Molecular connection between electrodes has been challenging the world since the concept of molecular electronics emergence in 1950s, and practical devices have remained elusive. Guo et al. made the breakthrough by covalently bonding a diarylethene molecule to graphene electrodes and achieved stable photoswitching at room temperature.

三明治结构MOFs催化剂:调控加氢反应选择性

刘鸣华

2017, 29 (1): 7-8 | DOI: 10.7536/PC170103

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摘要

This 2016 Chinese Chemistry Engram highlights the MOF catalyst for selective hydrogenation. The MOF catalyst is fabricated by sandwiching platinum nanoparticles between an inner core and an outer shell of an MOF with metal nodes of Fe³⁺, Cr³⁺ or both (known as MIL-101), which can convert a range of α, β-unsaturated aldehydes with high efficiency and with significantly enhanced selectivity towards unsaturated alcohols.

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