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Catalytic interconversion between hydrogen and formic acid at ambient temperature and pressure
Maenaka, Yuta,Suenobu, Tomoyoshi,Fukuzumi, Shunichi The Royal Society of Chemistry 2012 ENERGY AND ENVIRONMENTAL SCIENCE Vol.5 No.6
<P>Interconversion between hydrogen and formic acid in water at ambient temperature and pressure has been made possible by using a [C,N] cyclometalated organoiridium complex, [Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)benzoic acid-κ<I>C</I><SUP>3</SUP>)(H<SUB>2</SUB>O)]<SUB>2</SUB>SO<SUB>4</SUB> [<B>1</B>]<SUB>2</SUB>·SO<SUB>4</SUB>, as an efficient catalyst for both directions depending on pH. Hydrogenation of carbon dioxide by hydrogen occurs in the presence of a catalytic amount of <B>1</B> under an atmospheric pressure of H<SUB>2</SUB> and CO<SUB>2</SUB> in weakly basic water (pH 7.5) at room temperature, whereas formic acid efficiently decomposes to afford H<SUB>2</SUB> and CO<SUB>2</SUB> in the presence of <B>1</B> in acidic water (pH 2.8).</P> <P>Graphic Abstract</P><P>A [C,N] cyclometalated water-soluble iridium aqua complex acts as an efficient catalyst for interconversion between H<SUB>2</SUB> and HCOOH at ambient temperature and pressure in water by controlling pH. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c2ee03315a'> </P>
Maenaka, Yuta,Suenobu, Tomoyoshi,Fukuzumi, Shunichi American Chemical Society 2012 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.134 No.22
<P>A [C,N] cyclometalated Ir complex, [Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)benzoic acid-κ<I>C</I><SUP>3</SUP>)(H<SUB>2</SUB>O)]<SUB>2</SUB>SO<SUB>4</SUB> [<B>1</B>]<SUB>2</SUB>·SO<SUB>4</SUB>, was reduced by aliphatic alcohols to produce the corresponding hydride complex [Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)-benzoate-κ<I>C</I><SUP>3</SUP>)H]<SUP>−</SUP><B>4</B> at room temperature in a basic aqueous solution (pH 13.6). Formation of the hydride complex <B>4</B> was confirmed by <SUP>1</SUP>H and <SUP>13</SUP>C NMR, ESI MS, and UV–vis spectra. The [C,N] cyclometalated Ir-hydride complex <B>4</B> reacts with proton to generate a stoichiometric amount of hydrogen when the pH was decreased to pH 0.8 by the addition of diluted sulfuric acid. Photoirradiation (λ > 330 nm) of an aqueous solution of the [C,N] cyclometalated Ir-hydride complex <B>4</B> resulted in the quantitative conversion to a unique [C,C] cyclometalated Ir-hydride complex <B>5</B> with no byproduct. The complex <B>5</B> catalyzed hydrogen evolution from ethanol in a basic aqueous solution (pH 11.9) under ambient conditions. The 1,4-selective catalytic hydrogenation of β-nicotinamide adenine dinucleotide (NAD<SUP>+</SUP>) by ethanol was also made possible by the complex <B>1</B> to produce 1,4-dihydro-β-nicotinamide adenine dinucleotide (1,4-NADH) at room temperature. The overall catalytic mechanism of hydrogenation of NAD<SUP>+</SUP>, accompanied by the oxidation of ethanol, was revealed on the basis of the kinetic analysis and detection of the reaction intermediates.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2012/jacsat.2012.134.issue-22/ja302788c/production/images/medium/ja-2012-02788c_0011.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja302788c'>ACS Electronic Supporting Info</A></P>
Maenaka, Yuta,Suenobu, Tomoyoshi,Fukuzumi, Shunichi American Chemical Society 2012 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.134 No.1
<P>Regioselective hydrogenation of the oxidized form ofβ-nicotinamideadenine dinucleotide (NAD<SUP>+</SUP>) to the reduced form (NADH)with hydrogen (H<SUB>2</SUB>) has successfully been achieved in thepresence of a catalytic amount of a [C,N] cyclometalated organoiridiumcomplex [Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)benzoic acid-κ<I>C</I><SUP>3</SUP>)(H<SUB>2</SUB>O)]<SUB>2</SUB> SO<SUB>4</SUB> [<B>1</B>]<SUB>2</SUB>·SO<SUB>4</SUB> under an atmospheric pressure ofH<SUB>2</SUB> at room temperature in weakly basic water. The structureof the corresponding benzoate complex Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)-benzoate-κ<I>C</I><SUP>3</SUP>)(H<SUB>2</SUB>O) <B>2</B> has been revealedby X-ray single-crystal structure analysis. The corresponding iridiumhydride complex formed under an atmospheric pressure of H<SUB>2</SUB> undergoes the 1,4-selective hydrogenation of NAD<SUP>+</SUP> toform 1,4-NADH. On the other hand, in weakly acidic water the complex <B>1</B> was found to catalyze the hydrogen evolution from NADH toproduce NAD<SUP>+</SUP> without photoirradiation at room temperature.NAD<SUP>+</SUP> exhibited an inhibitory behavior in both catalytichydrogenation of NAD<SUP>+</SUP> with H<SUB>2</SUB> and H<SUB>2</SUB> evolution from NADH due to the binding of NAD<SUP>+</SUP> to thecatalyst. The overall catalytic mechanism of interconversion betweenNADH and NAD<SUP>+</SUP> accompanied by generation and consumptionof H<SUB>2</SUB> was revealed on the basis of the kinetic analysisand detection of the catalytic intermediates.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2012/jacsat.2012.134.issue-1/ja207785f/production/images/medium/ja-2011-07785f_0008.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja207785f'>ACS Electronic Supporting Info</A></P>
Nakajima Nozumu,Maenaka Takahiro,Kano Hiroki 대한척추외과학회 2020 Asian Spine Journal Vol.14 No.5
Study Design: Retrospective analysis of a case series of prospectively collected data. Purpose: To compare clinical and radiological outcomes between two posterior lumbar interbody fusion techniques: cortical bone trajectory (CBT) and traditional pedicle screw (PS).Overview of Literature: Biomechanical studies have revealed the benefits of the CBT technique. However, clinical evidence obtained from the direct comparison of outcomes between CBT and PS is limited.Methods: We retrospectively investigated 104 patients who had undergone posterior lumbar interbody fusion using CBT or PS. Clinical symptoms were evaluated and compared between CBT and PS using the Japanese Orthopedic Association Back Pain Evaluation Questionnaire (JOABPEQ) and Visual Analog Scale (VAS) before and 1 year after surgery. Spinal fusion status was assessed by multiplanar reconstruction computed tomography at 1 year after surgery.Results: The CBT and PS techniques were performed on 36 and 68 patients, respectively. Both CBT- and PS-treated patients exhibited improvement in each subdomain of the JOABPEQ and in the VAS. With regard to postoperative improvement of low back pain, the treatment effect, as assessed by the JOABPEQ, was greater for PS than for CBT. The spinal fusion rate was slightly lower for CBT than for PS, although the difference between them was not significant. The effect of treatment on postoperative low back pain was smaller for CBT than for PS, regardless of whether rigid spinal fusion was achieved.Conclusions: Clinical symptoms and spinal fusion efficiency were not significantly different between CBT and PS except for postoperative improvement in low back pain. The treatment effect on postoperative low back pain was smaller for CBT than for PS.
Radiation effects to acupuncture in mice embryos
Tano Kaori,Itokawa Yuka,Maenaka Toshihiro,Sakazaki Takahiko,Yamashita Takenori,Nakamura Takashi,Cho Kwang-Ho,Choi Jung-Sook,Ahn Kyoo-Seok,Ishida Torao,Gu Yeun-Hwa Kyung Hee Oriental Medicine Research Center 2006 Oriental pharmacy and experimental medicine Vol.6 No.3
We examined the radioprotection effects of acupoint (acupuncture point) stimulation during organogenesis stages of ICR mice. Pregnant mice received 1.5 Gy whole body X-irradiation on day 8 of gestation, which is the early stage of organogenesis. The embryonic death rate and teratogenesis rate by radiation were examined. Electroacupuncture to the leg acupoints and/ or transcutaneous stimulation to the back acupoints on the pregnant mice showed no protective effect against irradiation on embryonic or fetal death rate. On the contrary, the strong stimulation resulted in increase in the mortality after irradiation rather than protection. However acupoint stimulation to the pregnant mice never showed harmful effects by itself on embryos. It tended to reduce the skeletal malformations induced by X-ray irradiation. We suspect that acupoint stimulation removed the cells injured by irradiation during embryonic development, resulting in an increase in embryonic death rate and reduction in skeletal anomalies.
Antioxidant and immuno-enhancing effects of Echinacea purpurea (American herb) in vivo
Gu, Yeun-Hwa,Maenaka, Toshihiro,Saito, Kiyoto,Yamashita, Takenori,Choi, In-Suk,Terai, Kaoru,Ahn, Kyoo-Seok Kyung Hee Oriental Medicine Research Center 2005 Oriental pharmacy and experimental medicine Vol.5 No.1
We studied the protective effect of Echinacea purpurea against radiation by evaluating changes in the peripheral blood cell count and peripheral blood antioxidant activity. Echinacea purpurea administration had a suppressive effect on radiation-induced leukopenia, especially on lymphocytes and monocytes and resulted in a faster recovery of blood cell counts. Mouse peripheral blood antioxidant activity was increased by Echinacea purpurea, and a relationship between the suppressive effect on radiation-induced leukopenia and the antioxidant effect was suggested.
Damage of radioprotection and antitumor effects of water-soluble propolis
Terai, Kaoru,Ryu, Myung-Sun,Itokawa, Yuka,Maenaka, Toshihiro,Nakamura, Takashi,Hasegawa, Takeo,Choi, In-Suk,Ishida, Torao,Gu, Yeun-Hwa Kyung Hee Oriental Medicine Research Center 2006 Oriental pharmacy and experimental medicine Vol.6 No.1
Some natural products are able to inhibit radiation effects and exert an antitumor effect with fewer adverse reactions; however, their antitumor effects are less than those of widely-used synthetic drugs. Propolis is a natural material that has been attracting attention, and we extracted this material with water and investigated the effect of continuous propolis administration on radioactivity-induced reduction of hemocytes, in addition to the antioxidant and antitumor effects of propolis. Following a 1-week adjustment period, water-soluble propolis was administered intraperitoneally to male ICR mice at a dose of 100 mg/kg every other day for 2 weeks. Following administration, 2 Gy whole-body irradiation was performed and the counts of leukocytes, lymphocytes, and granulocytes and monocytes in the peripheral blood were determined 1, 3, 7, 15 and 30 days after irradiation. These cells were considered since they are closely associated with immunity to radioactivity. In a second experiment, water-soluble propolis was similarly administered to the mice for 2 weeks after a 1-week adjustment period, and 2 Gy whole-body irradiation was performed. The antioxidant effects in hemocytes were then investigated using 2,2'-azobis (2-amidinopropane) dihydrochloride (AAPH), a radical generator. In a third experiment, $1\;{\times}\;10^6$ Sarcoma-180 cells were inoculated into the right thigh of mice, which were divided into four groups: control, water-soluble propolis-treated, 6 Gy irradiated and water-soluble propolis-treated + 6 Gy irradiated groups, and changes in tumor size were measured for 20 days. Statistical analysis was conducted using ANOVA for multiple groups. In the three experiments, administration of water-soluble propolis inhibited the reduction of hemocytes caused by whole-body irradiation, showed antioxidant effects against radioactivity, and inhibited tumor growth, respectively. In conclusion, our data suggest that the antioxidant effect of watersoluble propolis inhibits hemocyte reduction caused by whole-body irradiation and enhances immunological inhibition of tumor growth.
Anti-tumor Immunity and Radioprotection Effect by Fuscoporia oblique
Yeunhwa Gu,Yuka Itokawa,Toshihiro Maenaka,Takenori Yamashita,Kenichiro Tanaka,Koru Tano,Hiroyo Kondo,Insuk Choi,Torao Ishida,Takashi Nakamura,Kiyoto Saito,Kaoru Terai,Hajime Monzen,Masami Oshima,Tetsu 한의병리학회 2005 대한동의병리학회 학술대회논문집 Vol.2005 No.8
Anti-rheumatoidal effects of Uncaria Tomentosa and Maytenus by a prolonged application
Choi, In-Sook,Yamashita, Takenori,Nakamura, Takashi,Maenaka, Toshihiro,Hasegawa, Takeo,Itokawa, Yuka,Ishida, Torao,Rhee, Juong-Gile,Gu, Yeun-Hwa Kyung Hee Oriental Medicine Research Center 2005 Oriental pharmacy and experimental medicine Vol.5 No.4
Uncaria Tomentosa and Maytenus are known to have anti-inflammatory and anti-rheumatoidal effects after either a single application or application over a short-term period. We applied these natural products to Wister rats every day for two weeks and investigated the effects of this long-term application on inflammation. This was done by measuring footpad edema, which was induced by a locally injected carrageenan. There was a dramatic reduction in edema in both U. Tomentosa- and Maytenus-treated rats; furthermore, the reduction lasted as long as three days for rats treated with U. Tomentosa. When the Balb/C mice underwent similar treatment for one month, the level of IgM in the blood of U. Tomentosa-treated mice decreased while the level of IgG in Maytenus-treated mice increased. This suggests that the long lasting effects of U. Tomentosa may be related to a low level of IgM and the subclass switch from IgM to IgG. Since the anti-inflammatory effects of U. Tomentosa lasts for three days, it may prove useful in treating rheumatoid arthritis when applied for an extended period of time, especially since this product is known to have minimal side effects.