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Hye Jin Shin,장윤정,Hikaru Zenno,Shinya Hayami,민길식 한국공업화학회 2022 Journal of Industrial and Engineering Chemistry Vol.110 No.-
Five polynuclear iron(III) complexes, [(pmidp)Fe(NCSe)]2 (1), [(pmidp)Fe(NCBH3)]2 (2), [(Hpmidp/pmidp)Fe3(CH3O)2(NCS)4]∙H2O (3), [(pmidp)2Fe6(CH3O)4(N3)4(CH3COO)2O2] (4), and[(pmidp)2Fe6(CH3O)4(NCO)4(CH3COO)2O2]∙2MeOH (5) were isolated through the reactions of N-(2-pyridylmethyl)iminodipropanol (H2pmidp) and iron(III) ions with different pseudohalide ions. The complexeswere studied via X-ray crystal diffraction, Mössbauer spectra, and magnetochemistry. The molecularstructures of 1 and 2 were formed as the {Fe2(m2-Opropoxo)2}2+ cores with pmidp2 and NCSe/NCBH3.The structure of 3 was formed as a {Fe3(m2-OCH3)2(m2-Opropoxo)4}5+ core with Hpmidp/pmidp2 andNCS. The structures of 4 and 5 were formed as {Fe6(m4-O)2(m2-OCH3)2(g2-OAc)2(m2-Opropoxo)4} cores withpmidp2 and NCO/N3. Structural analyses revealed that the formation of various multinuclear iron(III)moieties depends on the auxiliary ligands. The oxidation states of all the complexes were confirmedas + 3 using the bond valence sum (BVS) calculations and Mössbauer spectral data. The susceptibility datafor 1–5 fitted using each spin coupling (J) model indicated that 1–3 showed antiferromagnetic exchangeinteractions, and 4 and 5 showed the ferromagnetic and antiferromagnetic couplings, simultaneously.
Lee, Young Hoon,Kristopo, Hari,Woo, Arim,Won, Mi Seon,Hayami, Shinya,Thué,ry, Pierre,Jung, Ok-Sang,Lee, Hong In,Kim, Bok Jo,Lindoy, Leonard F.,Kim, Yang CSIRO Publishing 2012 Australian journal of chemistry Vol.65 No.7
<P> Two new polyamine ligands, L1 and L2, incorporating pyridyl and aliphatic amine donor sites have been prepared and their reaction with copper(ii) yields the mono- and binuclear complexes [Cu(L1)](ClO4)2 (1) and [Cl2Cu(L2)CuCl(H2O)]ClO4 (2), respectively. The X-ray structure of 1 confirms that the five nitrogen donors of L1 are bound to the central copper ion to give a distorted square pyramidal coordination sphere. In 2, L2 acts as a bridging ligand with its N3-donor coordination domains separated by a m-xylylene spacer group. An unusual feature of this latter complex is that symmetrical L2 gives rise to non-equivalent coordination behaviour at the individual copper sites; while both sites display five-coordination with distorted square pyramidal arrangements, they differ in having N3Cl2- and N3ClO-donor atom sets, respectively. The electron paramagnetic resonance (EPR) spectra of both complexes are discussed. Variable temperature magnetic susceptibility data confirmed the absence of magnetic interactions in 1 while a weak antiferromagnetic interaction between copper(ii) centres occurs in 2. </P>
Lee, Young Hoon,Shin, Jong Won,Sekimoto, Yusuke,Hayami, Shinya,Harrowfield, Jack,Kim, Yang Commonwealth Scientific and Industrial Research Or 2017 Australian journal of chemistry Vol.70 No.5
<P> Crystal structure determination on the mixed ligand complex [Ru(tpy)(L1)](ClO4)2 (tpy = 2,2′:6′,2″-terpyridine; L1 = 4′-(ferrocenylmethylaminomethylphenyl)terpyridine) shows the ferrocenyl group to be located as remotely as possible from the RuII centre. This may explain the fact that emission from the RuII centre is detectable even at room temperature in solution. </P>
Spin crossover in Co(<small>II</small>) metallorods – replacing aliphatic tails by aromatic
Lee, Young Hoon,Won, Mi Seon,Harrowfield, Jack M.,Kawata, Satoshi,Hayami, Shinya,Kim, Yang The Royal Society of Chemistry 2013 Dalton transactions Vol.42 No.32
<P>Terpyridine ligands with ter- and quater-phenyl substituents at the 4′ position provide bis(ligand)Co(<SMALL>II</SMALL>) complexes showing very different magnetic properties to those of their analogues with long-chain aliphatic substituents, with no evidence of “re-entrant” behavior involving multiple high- and low-spin species. Structure determinations of [Co(tptpy)<SUB>2</SUB>](BF<SUB>4</SUB>)<SUB>2</SUB>·CH<SUB>3</SUB>OH and [Co(qptpy)<SUB>2</SUB>](BPh<SUB>4</SUB>)<SUB>2</SUB>·3.5dmf·2H<SUB>2</SUB>O (dmf = <I>N</I>,<I>N</I>-dimethylformamide) show the metal ion centres in both to be relatively distant and that the “terpyridine embrace” observed to be partially retained in their analogues is completely lost. Consideration of available structural and magnetic data for these and other Co(<SMALL>II</SMALL>) complexes of functionalised terpyridines and terpyridine itself provides evidence that spin crossover behaviour may be regulated by face-to-face contacts of the pyridyl units of the head groups.</P> <P>Graphic Abstract</P><P>Spin crossover in Co(<SMALL>II</SMALL>) complexes of 4′-polyphenyl-terpyridines and their relatives appears to be regulated by face-to-face contacts of pyridyl units. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c3dt51396c'> </P>
Nakaya, Manabu,Ohtani, Ryo,Shin, Jong Won,Nakamura, Masaaki,Lindoy, Leonard F.,Hayami, Shinya The Royal Society of Chemistry 2018 Dalton Transactions Vol.47 No.39
<P>The cobalt(ii) complex incorporating π-conjugated substituent, [Co(Naph-C2-terpy)2](BF4)2 (1; Naph-C2-terpy = 4′-(2-naphthoxy(ethoxy))-2,2′:6′,2′′-terpyridine), exhibits an abrupt spin transition (ST) behavior (cooperative factor <I>C</I> = 0.91) while its solvated product, 1·2MeOH, shows gradual spin crossover (SCO) behavior (<I>C</I> = 0.49). Single crystal X-ray structural analyses demonstrated that the octahedral coordination core [CoN6] in 1 shows larger distortion in both high-spin and low-spin states than solvated 1·2MeOH or another two derivatives, [Co(R-terpy)2](BF4)2 (R = 2-naphthyl (2), 9-anthracenyl (3)). The respective distortion parameters (<I>Σ</I>) are compared with those for previously reported SCO cobalt(ii) compounds. The highly-distorted [CoN6] core in 1 (<I>Σ</I> = 126 in the HS state and 101.6 in the LS state) was stabilized by strong intermolecular interactions and observed an abrupt ST behaviour.</P>
Shin, Jong Won,Jeong, Ah Rim,Lee, Sun Young,Kim, Cheal,Hayami, Shinya,Min, Kil Sik The Royal Society of Chemistry 2016 Dalton transactions Vol.45 No.36
<P>The coordination chemistries of the tetradentate N2O2-type ligands N-(2-pyridylmethyl) iminodiethanol (H(2)pmide) and N-(2-pyridylmethyl) iminodiisopropanol (H(2)pmidip) have been investigated with nickel(II) and cobalt(II/III) ions. Three novel complexes prepared and characterized are [(Hpmide)(2)Ni-3(CH3COO)(4)] (1), [(Hpmide)(2)Co-3(CH3COO)(4)] (2), and [(pmidip)(2)Co-3(CH3COO)(4)] (3). In 1 and 2, two terminal nickel(II)/cobalt(II) units are coordinated to one Hpmide(-) and two CH3CO2-. The terminal units are each connected to a central nickel(II)/cobalt(II) cation through one oxygen atom of Hpmide(-) and two oxygen atoms of acetate ions, giving rise to nickel(II) and cobalt(II) trinuclear complexes, respectively. Trinuclear complexes 1 and 2 are isomorphous. In 3, two terminal cobalt(III) units are coordinated to pmidip(2-) and two CH3CO2-. The terminal units are each linked to a central cobalt(II) cation through two oxygen atoms of pmidip(2-) and one oxygen atom of a bidentate acetate ion, resulting in a linear trinuclear mixed-valence cobalt complex. 1 shows a weak ferromagnetic interaction with the ethoxo and acetato groups between the nickel(II) ions (g = 2.24, J = 2.35 cm(-1)). However, 2 indicates a weak antiferromagnetic coupling with the ethoxo and acetato groups between the cobalt(II) ions (g = 2.37, J = -0.5 cm(-1)). Additionally, 3 behaves as a paramagnetic cobalt(II) monomer, due to the diamagnetic cobalt(III) ions in the terminal units (g = 2.53, vertical bar D vertical bar= 36.0 cm(-1)). No catalytic activity was observed in 1. However, 2 and 3 showed significant catalytic activities toward various olefins with modest to good yields. 3 was slightly less efficient toward olefin epoxidation reaction than 2. Also 2 was used for terminal olefin oxidation reaction and was oxidised to the corresponding epoxides in moderate yields (34-75%) with conversions ranging from 47-100%. The cobalt complexes 2 and 3 promoted the O-O bond cleavage to similar to 75% heterolysis and similar to 25% homolysis.</P>
Soyoung Jeon,Yuri Jeong,Le Ngoc Tram Anh,Jeyun Ju,Daeheum Cho,Yoon Jung Jang,Ryuya Tokunaga,Shinya Hayami,Kil Sik Min 한국공업화학회 2023 Journal of Industrial and Engineering Chemistry Vol.128 No.-
In this work, we report novel enantiopure mononuclear complexes (teaH)[Ln((S,S)-dnsalcd)2] and (teaH)[Ln((R,R)-dnsalcd)2] (Ln = Eu3+ for 1 and 4, Tb3+ for 2 and 5, and Sm3+ for 3 and 6), where teaH = triethylammonium and (S,S/R,R)-H2dnsalcd = (S,S/R,R)-N,N’-bis(3,5-dinitrosalicylidene)-1,2-cyclohexanediamine. Their unique structural features have been studied by single crystal diffraction and chiral and magneticproperties have been investigated by circular dichroism and susceptibility, respectively. Notably, 1and 3 were found to be isomorphous and exhibited a single intramolecular p-p interaction between two(S,S)-dnsalcd2- ligands. In contrast, 2 and 5 were found to be isomorphous and displayed two intramolecularp-p interactions between two (S,S/R,R)-dnsalcd2- ligands. Interestingly, strong Eu3+/Sm3+-basedemissions in the solid and solution states were observed by efficient antenna effects due to the p-p interactionmodes of the coordinated ligands. Furthermore, density functional theory calculations indicatedthat 1 contained a single localized benzene group in the highest occupied molecular orbital (HOMO),whereas 2 exhibited full delocalization via p-p interactions in the HOMO.
The Impact of Neoadjuvant Chemotherapy for Borderline Resectable Pancreatic Cancer
( Manabu Kawai ),( Seiko Hirono ),( Ken-ichi Okada ),( Motoki Miyazawa ),( Yuji Kitahata ),( Ryohei Kobayashi ),( Masaki Ueno ),( Shinya Hayami ),( Hiroki Yamaue ) 대한간학회 2018 춘·추계 학술대회 (KASL) Vol.2018 No.1
Backgrounds: According to the National Comprehensive Cancer Network (NCCN) Clinical Practice Guidelines, pancreatic ductal adenocarcinoma (PDAC) can be classified as resectable, borderline resectable, or unresectable. Although borderline resectable PDAC (BRPC) may technically be resectable, it has particularly high risks of margin-positive resection and postoperative recurrence. Therefore, preoperative treatment is recommended for BRPC patients in both the NCCN Guidelines and an expert consensus statement. However, the establishment of the most appropriate neoadjuvant therapy is needed by further studies. The aim of these studies is to evaluate the impact of neoadjuvant chemotherapy for BRPC and confirm the safety and efficacy of two regimens of neoadjuvant therapy for BRPC. Our Clinical Trials: First, we evaluated the impact of neoadjuvant chemotherapy for BRPC. 143 BRPC-A patients undergoing pancreatectomy were reviewed from among 330 pancreatic cancer patients, including 111 potentially resectable pancreatic cancer patients and 76 BRPC with portal vein involvement patients. We compared the clinicopathological factors of 40 BRPC-A patients treated with neoadjuvant treatment followed by surgery and those of 103 BRPC-A patients treated with upfront surgery. The R0 rate and progression-free survival of BRPC-A patients who received neoadjuvant therapy and subsequent surgical resection were significantly better compared to those who received upfront surgery (R0: P = 0.041; progression-free survival: P = 0.033), but overall survival was not significantly different. Neoadjuvant treatment followed by surgery might provide clinical benefits for BRPC-A patients; however, the establishment of the most appropriate neoadjuvant treatment is needed by further studies. To evaluate appropriate neoadjuvant treatment, two prospective pilot trials were conducted as follows; modified FOLFIRINOX (without bolus 5-FU and LV, also decreased the dose of irinotecan; FIRINOX) and nab-paclitaxel plus gemcitabine therapy. Modified FOLFIRINOX was given to the first five patients in the 4-cycle group of the regimen and next five patients in the 8-cycle group. The primary end point was the toxicity of the therapy and one of the secondary end points were the optimal duration. The overall rate of grade 3 and 4 events was 80 %: 3 patients (60%) in the four-cycle group and five patients (100%) in the eight-cycle group had grade 3 or 4 adverse events. There was no incidence of serious adverse effect such as febrile neutropenia, sepsis, liver abscess or uncontrollable diarrhea. There was no clinically relevant morbidity presented in patients who underwent surgery. R0 rates by intention to treat were 60.0% in the four-cycle group and 40 % in the eight-cycle group (P = 0.999). The histopathologic treatment effect based on the Evans grade revealed grade I (n = 1), IIa (n = 3) in the four-cycle group and grade I (n = 2), IIa (n = 1) in the eight-cycle group. Nab-paclitaxel plus gemcitabine therapy: the primary endpoint was the toxicity, and secondary endpoints were the resection rate, the R0 resection rate. The overall rate of any grade and grade 3-4 events were 100% and 90%. The majority of these adverse events represented expected neutropenia. The resection and R0 resection rates were 80% and 70%, respectively. Conclusion: FIRINOX therapy was feasible and safe for strictly selected patients with BRPC. On the other hand, nab-paclitaxel plus gemcitabine therapy was safe and feasible without strict selection of patients with BRPC. A multicenter phase II study is in progress to investigate the efficacy of neoadjuvant nab-paclitaxel plus gemcitabine therapy on overall survival (UMIN000024154).