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通过钨对镍活性位点的电子改性实现苯甲胺选择性氧化耦合制氢
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作者 屠振涛 何晓洋 +5 位作者 刘璇 熊登科 左娟 吴德礼 汪建营 陈作锋 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第3期146-156,共11页
苯甲腈(BN)作为精细化学品、农用化学品和药品生产的重要中间体,其制备受到研究人员的广泛关注.传统的BN化学合成涉及有机物与氰化物之间的亲核取代反应.然而,由于氰化物等剧毒化学试剂的使用,这一反应在实际应用中受到了一定的限制.最... 苯甲腈(BN)作为精细化学品、农用化学品和药品生产的重要中间体,其制备受到研究人员的广泛关注.传统的BN化学合成涉及有机物与氰化物之间的亲核取代反应.然而,由于氰化物等剧毒化学试剂的使用,这一反应在实际应用中受到了一定的限制.最近研究发现,苯甲胺(BA)电化学氧化可为BN的生产提供一种清洁、高效、高选择性的方法.此外,与析氧反应(OER)相比,苯甲胺氧化反应(BAOR)具有明显的热力学优势;将BAOR与阴极析氢反应(HER)耦合,可提高整体电解体系的能效和经济效益.因此,开发高效双功能电催化剂用于苯甲胺氧化及耦合析氢反应具有重要的基础研究意义和实际应用价值.本文通过直接水热和高温磷化的方法,在泡沫镍基底上负载了一种W-Ni_(2)P纳米片(W-Ni_(2)P/NF),并探索了其作为双功能电催化剂在BAOR和HER的应用.实验结果显示,催化剂的纳米片结构不仅提供了充足的活性位点,还有助于离子传输.钨的掺杂显著增强了电化学传导性,改善了水吸附性,并优化了氢吸附能,进而提升了催化剂的HER性能.此外,钨的引入促进了电子从镍向钨的转移,形成了缺电子的镍区域;在W-Ni_(2)P催化的BAOR过程中,缺电子的镍活性位点与供电子的氨基(-NH2)相互作用,有效促进了氨基的吸附和活化,进一步推动了脱氢反应和C≡N键的形成.电化学测试结果表明,在1 mol L^(‒1)KOH溶液中,W-Ni_(2)P催化剂发生HER的过电位为80 mV(10 mA cm^(-2)),其性能可与商业Pt/C电极相媲美.在含有25 mmol L^(‒1)BA的1 mol L^(‒1)KOH溶液中,仅需施加1.42 V电位,W-Ni_(2)P催化剂即可达到100 mA cm^(-2)的氧化电流密度,这比OER所需电位低350 mV.此外,当组装W-Ni_(2)P/NF||W-Ni_(2)P/NF电解槽时,在1 mol L^(‒1)KOH和25 mmol L^(‒1)BA的电解液中,仅需1.41 V的电解电压即可达到10 mA cm^(-2)的电流密度,实现了阴极制氢和阳极增值BN的同时生产,且反应的法拉第效率达到95%.采用电化学原位拉曼光谱和红外光谱研究了反应的活性位点和关键中间产物.结合密度泛函理论计算,阐明了BAOR的催化机理以及反应路径,深入分析了W掺杂在优化吸附能和提高W-Ni2P电催化剂催化活性方面的优化作用.综上所述,本文成功制备了高活性、高稳定性的钨掺杂磷化镍纳米片双功能催化剂,并将其应用于两电极电解体系中,实现了阴、阳极高附加值产物(苯甲腈和氢气)的同时生成.本研究为电化学合成高价值腈化合物和制氢先进催化剂的设计、制备提供了一定的参考和借鉴. 展开更多
关键词 双功能电催化剂 选择性氧化 苯甲腈电合成 脱氢作用 析氢反应
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Assessing the current situation and the influencing factors affecting perceived stigma among older patients after leukemia diagnosis
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作者 Xuan Tang Shuang-Qin Chen +3 位作者 Jiang-Hua Huang Cai-Feng Deng Jie-Qiong Zou juan zuo 《World Journal of Psychiatry》 SCIE 2024年第6期812-821,共10页
BACKGROUND Psychological problems are becoming increasingly prominent among older patients with leukemia,with patients potentially facing stigmatization after diagnosis.However,there is limited research on the stigma ... BACKGROUND Psychological problems are becoming increasingly prominent among older patients with leukemia,with patients potentially facing stigmatization after diagnosis.However,there is limited research on the stigma experienced by these patients and the factors that may contribute to it.AIM To investigate the stigma faced by older patients after being diagnosed with leukemia and to analyze the potential influencing factors.METHODS A retrospective analysis was conducted using clinical data obtained from questionnaire surveys,interviews,and the medical records of older patients with leukemia admitted to the Hengyang Medical School from June 2020 to June 2023.The data obtained included participants’basic demographic information,medical history,leukemia type,family history of leukemia,average monthly family income,pension,and tendency to conceal illness.The Chinese versions of the Social Impact Scale(SIS),Perceived Social Support Scale(PSSS),Self-Rating Anxiety Scale(SAS),and Self-Rating Depression Scale(SDS)were used to assess indicators related to stigma,social support,and mental health status.We used Pearson’s correlation coefficient to analyze the strength and direction of the relationship between the scores of each scale,and regression analysis to explore the factors related to the stigma of older patients with leukemia after diagnosis.RESULTS Data from 120 patients with leukemia aged 65-80 years were analyzed.The total score on the SIS and PSSS was 43.60±4.07 and 37.06±2.87,respectively.The SAS score was 58.35±8.32 and the SDS score was 60.58±5.97.The stigma experienced by older leukemia patients was negatively correlated with social support(r=-0.691,P<0.05)and positively correlated with anxiety and depression(r=0.506,0.382,P<0.05).Age,education level,smoking status,average monthly family income,pension,and tendency to conceal illness were significantly associated with the participants’level of stigma(P<0.05).Age,smoking status,social support,anxiety,and depression were predictive factors of stigmatization among older leukemia patients after diagnosis(all P<0.05),with a coefficient of determination(R2)of 0.644 and an adjusted R2 of 0.607.CONCLUSION Older patients commonly experience stigmatization after being diagnosed with leukemia.Factors such as age,smoking status,social support,and psychological well-being may influence older patients’reported experience of stigma. 展开更多
关键词 Senile leukemia STIGMA Social support ANXIETY DEPRESSION Influencing factors
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