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Brumm, S.*; Gabrielli, F.*; Sanchez Espinoza, V.*; Stakhanova, A.*; Groudev, P.*; Petrova, P.*; Vryashkova, P.*; Ou, P.*; Zhang, W.*; Malkhasyan, A.*; et al.
Annals of Nuclear Energy, 211, p.110962_1 - 110962_16, 2025/02
被引用回数：1 パーセンタイル：0.00(Nuclear Science & Technology)The completed Horizon-2020 project on "Management and Uncertainties of Severe Accidents (MUSA)" has reviewed uncertainty sources and Uncertainty Quantification methodology for the purpose of assessing Severe Accidents (SA). The key motivation of the project has been to bring the advantages of the Best Estimate Plus Uncertainty approach to the field of Severe Accident. The applications brought together a large group of participants that set out to apply uncertainty analysis (UA) within their field of SA modelling expertise, in particular reactor types, but also SA code used (ASTEC, MELCOR, etc.), uncertainty quantification tools used (DAKOTA, RAVEN, etc.), detailed accident scenarios, and in some cases SAM actions. This paper synthesizes the reactor-application work at the end of the project. Analyses of 23 partners are sorted into different categories, depending on whether their main goal is/are (i) uncertainty bands of simulation results; (ii) the understanding of dominating uncertainties in specific sub-models of the SA code; (iii) improving the understanding of specific accident scenarios, with or without the application of SAM actions; or, (iv) a demonstration of the tools used and developed, and of the capability to carry out an uncertainty analysis in the presence of the challenges faced. The partners' experiences made during the project have been evaluated and are presented as good practice recommendations. The paper ends with conclusions on the level of readiness of UA in SA modelling, on the determination of governing uncertainties, and on the analysis of SAM actions.
Che, G.*; Fei, Y.*; Tang, X.*; Zhao, Z.*; 服部 高典; 阿部 淳*; Wang, X.*; Ju, J.*; Dong, X.*; Wang, Y.*; et al.
Physical Chemistry Chemical Physics, 27(2), p.1112 - 1118, 2025/01
芳香族分子の圧力誘起重合(PIP)は、様々な炭素系材料を合成するための効果的な方法として浮上してきた。目的とする構造や機能を得るためには、適切な官能基化された分子前駆体の選択が極めて重要である。本研究では、1,4-ジフルオロベンゼン(1,4-DFB)をPIPの構成要素として選択した。1,4-DFBをその場高圧で調べた結果、約12.0GPaで相転移が起こり、18.7GPaで不可逆的な化学反応が起こることがわかった。生成物の構造解析と反応のカイネティクスから、直線的な成長を伴う擬六方晶積層フッ素ダイヤモンドナノスレッドの形成が明らかになった。高圧下のベンゼンの結晶構造と比較して、1,4-DFBは[001]軸に沿って高い圧縮を示す。この異方的な圧縮は、[01
]軸に沿ったより強いH
相互作用と、[100]軸と[010]軸に沿った潜在的な圧縮阻害H
F相互作用に起因し、[01]軸に沿った可能な反応経路を促進する。この研究は、分子スタッキングを調節し、反応経路に影響を与える官能基化の重要な役割を強調している。
Zheng, X.-G.*; 山内 一宏*; 萩原 雅人; 西堀 英治*; 河江 達也*; 渡邊 功雄*; 内山 智貴*; Chen, Y.*; Xu, C.-N.*
Nature Communications (Internet), 15, p.9989_1 - 9989_12, 2024/11
被引用回数：0Like the crystallization of water to ice, magnetic transition occurs at a critical temperature after the slowing down of dynamically fluctuating short-range correlated spins. Here, we report a unique type of magnetic transition characterized by a linear increase in the volume fraction of unconventional static short-range-ordered spin clusters, which triggered a transition into a long-range order at a threshold fraction perfectly matching the bond percolation theory in a new quantum antiferromagnet of pseudo-trigonal Cu
(OH)
Cl
. Static short-range order appeared in its Kagome lattice plane below Ca. 20 K from a pool of coexisting spin liquid, linearly increasing its fraction to 0.492(8), then all Kagome spins transitioned into a stable two-dimensional spin order at 
_
_
_
_
$. The unconventional static nature of the short-range order was inferred to be due to a pinning effect by the strongly correlated coexisting spin liquids. This work presents a unique magnetic system to demonstrate a complete bond percolation process toward the critical transition. Meanwhile, the unconventionally developed magnetic order in this chemically clean system should shed new light on spin-liquid physics.
-
transitionsYang, Q.*; Yang, X.*; Wang, Y.*; Fei, Y.*; Li, F.*; Zheng, H.*; Li, K.*; Han, Y.*; 服部 高典; Zhu, P.*; et al.
Nature Communications (Internet), 15, p.7778_1 - 7778_9, 2024/09
被引用回数：0 パーセンタイル：0.00(Multidisciplinary Sciences)明るい一重項励起子と三重項励起子を同時に発現する発光材料は、オプトエレクトロニクス、サイネージ、情報暗号化において大きな可能性を秘めている。しかしながら、高性能の白色発光を実現するためには、蛍光と燐光の寄与が不均衡であることが大きな障害となっている。ここでは、水素結合の協同効果による圧力処理エンジニアリングによって、n--遷移の混合を実現し、イソフタル酸(IPA)中で三重項状態の発光を7%から40%に高めることで、この課題に対処した。加圧処理したIPAでは、蛍光と燐光のハイブリッドに基づく優れた白色発光が得られ、フォトルミネッセンス量子収率は当初の19%(青色発光)から75%に増加した。その場での高圧IRスペクトル、X線回折、中性子回折から、圧力の上昇に伴い水素結合が連続的に強化されることが明らかになった。さらに、この強化された水素結合は、圧力処理後も常圧条件下まで保持され、バランスの取れた一重項/三重項励起子集団のための効率的な系間交差を目的としたIPAに与え、効率的な白色発光をもたらした。この研究は、有機低分子の三重項状態を明るくするルートを提案するだけでなく、一重項励起子と三重項励起子の比率を調節して、高性能の白色発光を構築するものである。
Baccou, J.*; Glantz, T.*; Ghione, A.*; Sargentini, L.*; Fillion, P.*; Damblin, G.*; Sueur, R.*; Iooss, B.*; Fang, J.*; Liu, J.*; et al.
Nuclear Engineering and Design, 421, p.113035_1 - 113035_16, 2024/05
被引用回数：4 パーセンタイル：96.65(Nuclear Science & Technology)In the Best-Estimate Plus Uncertainty (BEPU) framework, the use of best-estimate code requires to go through a Verification, Validation and Uncertainty Quantification process (VVUQ). The relevance of the experimental data in relation to the physical phenomena of interest in the VVUQ process is crucial. Adequacy analysis of selected experimental databases addresses this problem. The outcomes of the analysis can be used to select a subset of relevant experimental data, to encourage designing new experiments or to drop some experiments from a database because of their substantial lack of adequacy. The development of a specific transparent and reproducible approach to analyze the relevance of experimental data for VVUQ still remains open and is the topic of this contribution. In this paper, the concept of adequacy initially introduced in the OECD/NEA SAPIUM (Systematic APproach for model Input Uncertainty quantification Methodology) activity is formalized. It is defined through two key properties, called representativeness and completeness, that allows considering the multifactorial dimension of the adequacy problem. A new systematic approach is then proposed to analyze the adequacy of a set of experimental databases. It relies on the introduction of two sets of criteria to characterize representativeness and completeness and on the use of multi-criteria decision analysis method to perform the analysis. Finally, the approach is applied in the framework of the new OECD/NEA ATRIUM activity which includes a set of practical IUQ exercises in thermal-hydraulics to test the SAPIUM guideline in determining input uncertainties and forward propagating them on an application case. It allows evaluating the adequacy of eight experimental databases coming from the Super Moby-dick, Sozzi-Sutherland and Marviken experiments and identifying the most adequate ones.
久保 光太郎; Zheng, X.; 田中 洋一; 玉置 等史; 杉山 智之; Jang, S.*; 高田 孝*; 山口 彰*
Proceedings of the Institution of Mechanical Engineers, Part O; Journal of Risk and Reliability, 237(5), p.947 - 957, 2023/10
被引用回数：5 パーセンタイル：61.27(Engineering, Multidisciplinary)確率論的リスク評価(Probabilistic Risk Assessment: PRA)は、大規模かつ複雑なシステムのリスクを評価するために用いられる手法である。しかし、従来のイベントツリーやフォールトツリーを用いたPRAでは、原子力発電所の構造物、系統及び機器が損傷するタイミングを考慮することは困難である。そこで、この課題を解決するために、RAPID(Risk Assessment with Plant Interactive Dynamics)を用いて、熱水力解析と外部事象のシミュレーションを組み合わせた手法を提案した。加圧水型原子炉のタービン建屋内での内部溢水を表現するために、ベルヌーイの定理に基づいた溢水伝播モデルを適用した。加えて、溢水源の流量や緩和システムの故障基準などの不確実さを考慮した。シミュレーションでは、運転員がいくつか簡略化を行うことにより、運転員による溢水源の隔離操作と排水ポンプを用いた回復操作をモデル化した。その結果、隔離と排水を組み合わせることで、溢水発生時の条件付炉心損傷確率を約90%低減できることが示された。
Zheng, X.*; 加藤 優*; 上村 洋平*; 松村 大樹; 八木 一三*; 高橋 仁徳*; 野呂 真一郎*; 中村 貴義*
Inorganic Chemistry, 62(3), p.1257 - 1263, 2023/01
被引用回数：6 パーセンタイル：80.27(Chemistry, Inorganic & Nuclear)A glass-crystal composite (g-NCP/PCP), comprising a glassy nonporous coordination polymer (g-NCP) and a crystalline porous coordination polymer (PCP)/metal-organic framework, was synthesized by using a melt-quenched method. Compared to that of the PCP itself, g-NCP/PCP has an enhanced gas adsorption selectivity. The results should stimulate further studies of the chemistry of g-NCP/PCP glass-crystal composites.
Zheng, X.; 玉置 等史; 高原 省五; 杉山 智之; 丸山 結
Proceedings of Probabilistic Safety Assessment and Management (PSAM16) (Internet), 10 Pages, 2022/09
Uncertainty gives rise to the risk. For nuclear power plants, probabilistic risk assessment (PRA) systematically concludes what people know to estimate the uncertainty in the form of, for example, risk triplet. Capable of developing a definite risk profile for decision-making under uncertainty, dynamic PRA widely applies explicit modeling techniques such as simulation to scenario generation as well as the estimation of likelihood/probability and consequences. When quantifying risk, however, epistemic uncertainties exist in both PRA and dynamic PRA, as a result of the lack of knowledge and model simplification. The paper aims to propose a practical approach for the treatment of uncertainty associated with dynamic PRA. The main idea is to perform the uncertainty analysis by using a two-stage nested Monte Carlo method, and to alleviate the computational burden of the nested Monte Carlo simulation, multi-fidelity models are introduced to the dynamic PRA. Multi-fidelity models include a mechanistic severe accident code MELCOR2.2 and machine learning models. A simplified station blackout (SBO) scenario was chosen as an example to show practicability of the proposed approach. As a result, while successfully calculating the probability of large early release, the analysis is also capable to provide uncertainty information in the form probability distributions. The approach can be expected to clarify questions such as how reliable are results of dynamic PRA.
Zheng, X.; 玉置 等史; 杉山 智之; 丸山 結
Reliability Engineering & System Safety, 223, p.108503_1 - 108503_12, 2022/07
被引用回数：19 パーセンタイル：86.11(Engineering, Industrial)Dynamic probabilistic risk assessment (PRA) more explicitly treats timing issues and stochastic elements of risk models. It extensively resorts to iterative simulations of accident progressions for the quantification of risk triplets including accident scenarios, probabilities and consequences. Dynamic PRA leverages the level of detail for risk modeling while intricately increases computational complexities, which result in heavy computational cost. This paper proposes to apply multi-fidelity simulations for a cost- effective dynamic PRA. It applies and improves the multi-fidelity importance sampling (MFIS) algorithm to generate cost-effective samples of nuclear reactor accident sequences. Sampled accident sequences are paralleled simulated by using mechanistic codes, which is treated as a high-fidelity model. Adaptively trained by using the high-fidelity data, low-fidelity model is used to predicting simulation results. Interested predictions with reactor core damages are sorted out to build the density function of the biased distribution for importance sampling. After when collect enough number of high-fidelity data, risk triplets can be estimated. By solving a demonstration problem and a practical PRA problem by using MELCOR 2.2, the approach has been proven to be effective for risk assessment. Comparing with previous studies, the proposed multi-fidelity approach provides comparative estimation of risk triplets, while significantly reduces computational cost.
Brumm, S.*; Gabrielli, F.*; Sanchez-Espinoza, V.*; Groudev, P.*; Ou, P.*; Zhang, W.*; Malkhasyan, A.*; Bocanegra, R.*; Herranz, L. E.*; Berda
, M.*; et al.
Proceedings of 10th European Review Meeting on Severe Accident Research (ERMSAR 2022) (Internet), 13 Pages, 2022/05
The current HORIZON-2020 project on "Management and Uncertainties of Severe Accidents (MUSA)" aims at applying Uncertainty Quantification (UQ) in the modeling of Severe Accidents (SA), particularly in predicting the radiological source term of mitigated and unmitigated accident scenarios. Within its application part, the project is devoted to the uncertainty quantification of different severe accident codes when predicting the radiological source term of selected severe accident sequences of different nuclear power plant designs, e.g. PWR, VVER, and BWR. Key steps for this investigation are, (a) the selection of severe accident sequences for each reactor design, (b) the development of a reference input model for the specific design and SA-code, (c) the selection of a list of uncertain model parameters to be investigated, (d) the choice of an UQ-tool e.g. DAKOTA, SUSA, URANIE, etc., (e) the definition of the figures of merit for the UA-analysis, (f) the performance of the simulations with the SA-codes, and, (g) the statistical evaluation of the results using the capabilities, i.e. methods and tools offered by the UQ-tools. This paper describes the project status of the UQ of different SA codes for the selected SA sequences, and the technical challenges and lessons learnt from the preparatory and exploratory investigations performed.
Wang, X.*; Tang, X.*; Zhang, P.*; Wang, Y.*; Gao, D.*; Liu, J.*; Hui, K.*; Wang, Y.*; Dong, X.*; 服部 高典; et al.
Journal of Physical Chemistry Letters (Internet), 12(50), p.12055 - 12061, 2021/12
被引用回数：10 パーセンタイル：62.66(Chemistry, Physical)置換ポリアセチレンは、ポリアセチレン骨格の化学的安定性,物性,付加機能の向上が期待されるが、その多様性は非常に限られている。今回我々は、固体のアセチレンジカルボン酸に外圧を加えることにより、従来の方法では合成が非常に困難であったトランス-ポリアセチレン骨格上のすべての炭素がカルボキシル基に結合した結晶性のポリ-ジカルボキシルアセチレンができることを報告する。重合は、水素結合を利用したトポケミカル反応であった。このユニークな構造は、カルボニル基の極めて高い含有量とポリアセチレン骨格の高い導電性を組み合わせたもので、リチウムイオン電池(LIB)負極として高い比容量と優れたサイクル/レート性能を示す。我々は、完全に機能化された結晶性ポリアセチレンを紹介し、高分子LIB材料や活性基を多く含む高分子材料合成のために圧力重合が有力な方法であることを提案する。
Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; 服部 高典; Wang, Y.*; Dong, X.*; et al.
Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09
被引用回数：5 パーセンタイル：27.31(Chemistry, Physical)窒素に富む分子の圧力有機相転移や重合は、環境にやさしい高エネルギー密度材料の開発にとって非常に重要であるため、広く注目されている。本論文では、その場ラマン,IR,X線回折,中性子回折、および理論計算をもちい、100GPaまでの1H-テトラゾールの相転移挙動と化学反応の研究を紹介する。2.6GPa以上での相転移が確認され、その高圧構造は、以前に報告されたユニットセル内に2つの分子をもつものではなく、1つの分子をものであることが分かった。1H-テトラゾールは、おそらく窒素-窒素結合ではなく炭素-窒素結合により、100GPa以下で可逆的に重合する。私たちの研究は、1H-テトラゾールの高圧相の構造モデルを更新し、もっともらしい分子間結合の経路を初めて提示した。これにより、窒素に富む化合物の相転移と化学反応の理解が進み、新しい高エネルギー密度材料の設計に役立つと考えられる。
Hao, Y. Q.*; Wo, H. L.*; Gu, Y. M.*; Zhang, X. W.*; Gu, Y. Q.*; Zheng, S. Y.*; Zhao, Y.*; Xu, G. Y.*; Lynn, J. W.*; 中島 健次; et al.
Science China; Physics, Mechanics & Astronomy, 64(3), p.237411_1 - 237411_6, 2021/03
被引用回数：11 パーセンタイル：70.28(Physics, Multidisciplinary)We report thermodynamic and neutron diffraction measurements on the magnetic ordering properties of the honeycomb lattice magnet YbCl. We find YbCl exhibits a N
el type long-range magnetic order at the wavevector (0, 0, 0) below T
= 600 mK. This magnetic order is associated with a small sharp peak in heat capacity and most magnetic entropy release occurs above the magnetic ordering temperature. The magnetic moment lies in-plane, parallel to the monoclinic a-axis, whose magnitude m
= 0.86(3) 
is considerably smaller than the expected fully ordered moment of 2.24 for the doublet crystal-field ground state. The magnetic ordering moment gradually increases with increasing magnetic field perpendicular to the ab-plane, reaching a maximum value of 1.6(2) at 4 T, before it is completely suppressed above 
9 T. These results indicate the presence of strong quantum fluctuations in YbCl.
Wang, Y.*; Jia, G.*; Cui, X.*; Zhao, X.*; Zhang, Q.*; Gu, L.*; Zheng, L.*; Li, L. H.*; Wu, Q.*; Singh, D. J.*; et al.
Chem, 7(2), p.436 - 449, 2021/02
被引用回数：251 パーセンタイル：99.77(Chemistry, Multidisciplinary)Nanozymes are promising alternatives to natural enzymes, but their use remains limited owing to poor specificity. Overcoming this is extremely challenging due to the intrinsic structural complexity of these systems. We report theoretical design and experimental realization of a series of heterogeneous molybdenum single-atom nanozymes (named Mo
-N
-C), wherein we find that the peroxidase-like specificity is well regulated by the coordination numbers of single Mo sites. The resulting Mo-N
-C catalyst shows exclusive peroxidase-like behavior. It achieves this behavior via a homolytic pathway, whereas Mo-N-C and Mo-N-C catalysts have a different heterolytic pathway. The mechanism of this coordination-number-dependent enzymatic specificity is attributed to geometrical structure differences and orientation relationships of the frontier molecular orbitals.
Lai, W.-H.*; Wang, H.*; Zheng, L.*; Jiang, Q.*; Yan, Z.-C.*; Wang, L.*; 吉川 浩史*; 松村 大樹; Sun, Q.*; Wang, Y.-X.*; et al.
Angewandte Chemie; International Edition, 59(49), p.22171 - 22178, 2020/12
被引用回数：92 パーセンタイル：95.69(Chemistry, Multidisciplinary)Herein, we report a comprehensive strategy to synthesize a full range of single-atom metals on carbon matrix, including V, Mn, Fe, Co, Ni, Cu, Ge, Mo, Ru, Rh, Pd, Ag, In, Sn, W, Ir, Pt, Pb, and Bi. The extensive applications of various single-atom catalysts (SACs) are manifested via their ability to electro-catalyze typical hydrogen evolution reactions (HER) and conversion reactions in novel room-temperature sodium sulfur batteries (RT-Na-S). The enhanced performances for these electrochemical reactions arisen from the ability of different single active atoms on local structures to tune their electronic configuration. Significantly, the electrocatalytic behaviors of diverse SACs, assisted by density functional theory calculations, are systematically revealed by in situ synchrotron X-ray diffraction and in situ transmission electronic microscopy, providing a strategic library for the general synthesis and extensive applications of SACs in energy conversion and storage.
Zheng, X.; Mandelli, D.*; Alfonsi, A.*; Smith, C.*; 杉山 智之
Proceedings of 30th European Safety and Reliability Conference and 15th Probabilistic Safety Assessment and Management Conference (ESREL 2020 and PSAM-15) (Internet), p.2176 - 2183, 2020/11
The paper introduces a simulation-based Level 2 probabilistic risk assessment (PRA) of a multi-unit nuclear power plant. We propose the methodology by quantifying risk for a station-blackout accident scenario, initialized by a loss-of-offsite-power event. Contrary to classical PRA that applies static models such as event-tree/fault-tree, the analysis is seamlessly integrated with mechanistic simulation and PRA models, including: (1) a simplified thermal-hydraulic code for simulating system behaviors; (2) a Markovian model for the failure mechanism of decay-heat-removal systems, to investigate the interaction between mechanistic simulation and reliability analysis; and (3) classical containment event trees for evaluating containment performances and hydrogen-explosion risk under severe accident conditions. All dynamic and static models, including plant dependencies, are unified within the RAVEN computational framework, applying RAVEN components, External Model, Ensemble Model, and PRA Plugins. The study demonstrates an integrated assessment of risks by considering accident progression and inter-unit system interactions, both time dependent. Statistical data analysis is used to quantifying risk metrics, including core damage frequencies, large early release frequencies and plant damage status. The methodology pertains to modern risk-analysis methodologies such as risk-informed safety margin characterization (RISMC) and dynamic PRA.
久保 光太郎; Zheng, X.; 田中 洋一; 玉置 等史; 杉山 智之; Jang, S.*; 高田 孝*; 山口 彰*
Proceedings of 30th European Safety and Reliability Conference and 15th Probabilistic Safety Assessment and Management Conference (ESREL 2020 and PSAM-15) (Internet), p.2279 - 2286, 2020/11
確率論的リスク評価(PRA)は巨大かつ複雑なシステムをリスクを評価する手法の1つである。従来のPRA手法を用いて外部事象のリスクを評価する場合、構造物、系統及び機器の機能喪失時刻の取扱いが困難である。この解決策として、熱水力解析と外部事象評価シミュレーションをRAPID (Risk Assessment with Plant Interactive Dynamics)コードを用いて結合した。外部事象としてPWRプラントにおけるタービン建屋内での内部溢水を選定し、溢水進展評価にはベルヌーイ則に式を用いた。また、溢水源の流量及び緩和設備の没水基準に関する不確実さを考慮した。回復操作については、運転員による溢水源の隔離とポンプによる排水を仮定とともにモデル化した。結果として、隔離操作が排水と組み合わせることによりより有効になることが示された。
田中 洋一; 玉置 等史; Zheng, X.; 杉山 智之
Proceedings of 30th European Safety and Reliability Conference and 15th Probabilistic Safety Assessment and Management Conference (ESREL 2020 and PSAM-15) (Internet), p.2195 - 2201, 2020/11
One advantage of dynamic probabilistic risk assessment (PRA) is that it can take into account the timing and ordering of event occurrences based on more explicit simulation of system dynamics. It is expected that dynamic PRA can lead us into a more realistic risk assessment, overcoming some limitations of conventional PRA. Multiple dynamic PRA tools have been developed worldwide, and applied to risk assessment of large industrial facilities such as nuclear power plants and crewed spacecrafts. Japan Atomic Energy Agency has developed the dynamic PRA tool, RAPID (Risk Assessment with Plant Interactive Dynamics), considering the interaction between accident simulation and dysfunctional models of safety-related systems. This paper introduces a recent enhancement of RAPID to treat more complicated simulation interactions from the outside of severe accident codes. It is designed to feed back and forth plant information from simulators to the accident sequence generator. It discusses how the enhancement affects the results of risk assessment, with an example analyzing thermal failure of a safety relief valve in a station blackout accident occurred at a boiling water reactor plant.
久保 光太郎; Zheng, X.; 石川 淳; 杉山 智之; Jang, S.*; 高田 孝*; 山口 彰*
Proceedings of Asian Symposium on Risk Assessment and Management 2020 (ASRAM 2020) (Internet), 11 Pages, 2020/11
動的確率論的リスク評価(PRA)は、従来のPRAよりも現実的で詳細な解析を可能とする。しかし、これらの改善とトレードオフの関係にあるのは、多数の熱水力解析を行うことに伴う膨大な計算コストである。本研究では、機械学習に基づいて、熱水力解析を省略することでこの計算コストを削減することを目指した。機械学習には、サポートベクターマシンを選択し、その構築には高忠実度・高コストの詳細モデルと、低忠実度・低コストの簡易モデルを用いた。その結果、今回仮定した条件においては、精度を大幅に低下させることなく計算コストを約80%削減することができた。
Zhang, P.*; Tang, X.*; Wang, Y.*; Wang, X.*; Gao, D.*; Li, Y.*; Zheng, H.*; Wang, Y.*; Wang, X.*; Fu, R.*; et al.
Journal of the American Chemical Society, 142(41), p.17662 - 17669, 2020/10
被引用回数：28 パーセンタイル：77.11(Chemistry, Multidisciplinary)固体トポケミカル重合(SSTP)は機能的な結晶性高分子材料を合成するための有望な方法であるが、溶液中で起こるさまざまな反応とは対照的に、非常に限られたタイプのSSTP反応しか報告されていない。ディールス・アルダー(DA)および脱水素-DA(DDA)反応は、溶液中で六員環を作るための教科書的反応であるが、固相合成ではほとんど見られない。本研究では、固体の1,4-ジフェニルブタジイン(DPB)を10-20GPaに加圧することで、フェニル基がジエノフィルとして、DDA反応することを複数の最先端の手法を用いて明らかにした。臨界圧力での結晶構造は、この反応が「距離選択的」であることを示している。つまり、フェニルとフェニルエチニル間の距離3.2
は、DDA反応は起こせるが、他のDDAや1,4-付加反応で結合を形成するには長すぎる。回収された試料は結晶性の肘掛け椅子型のグラファイトナノリボンであるため、今回の研究結果は、原子スケールの制御で結晶質炭素材料を合成するための新しい道を開く。
