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金屬有機框架材料對Cr(Ⅵ)離子的吸附去除研究進展
李茹霞, 鐘文彬, 謝林華, 謝亞勃, 李建榮
2021, 37(3): 385-400  doi: 10.11862/CJIC.2021.068
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摘要:
重金屬離子污染問題一直備受關注。開發利用多孔材料吸附去除水中重金屬離子一直是材料、環境等相關學科領域的研究熱點之一。金屬有機框架材料(metal-organic frameworks,MOFs)是一類新型的多孔材料,具有結構多樣、比表面積大、孔徑可調、孔表面特征易設計調控等特點,在氣體分離、催化、傳感等領域表現出極大的應用潛力。近年來,高穩定MOF材料的構筑取得了許多重大突破,大量研究工作探索了這類材料在水中的應用,包括水中重金屬離子的吸附去除。Cr(Ⅵ)離子是一類毒性大、分布廣的重金屬離子,不同條件下存在形態多樣,其吸附去除研究具有理論和實際意義。本文主要綜述了近年來利用MOF材料吸附去除水中Cr(Ⅵ)離子的研究工作,并將這些材料歸屬為:(1)高穩定的鋯基MOF、(2)陽離子框架型MOF、(3)后修飾的MOF及(4)MOF基復合材料4類;也對這些材料的Cr(Ⅵ)離子吸附機理、吸附量、材料再生性等進行了概括;最后分析了MOF材料在重金屬離子吸附去除實際應用上存在的問題并展望了今后的重點研究方向。
論文
基于粘度響應的線粒體靶向銥(Ⅲ)配合物用于腫瘤的光動力治療
歐陽艾, 羅雨珩, 陸農, 胡仁濤, 張平玉, 張黔玲
2021, 37(3): 401-411  doi: 10.11862/CJIC.2021.052
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合成了2種含有轉動基團的銥配合物Ir1Ir2。研究發現Ir1Ir2對粘度具有靈敏的熒光響應,在高粘度環境下,其熒光強度分別提高了35.7倍和1 311.6倍。細胞攝取和共定位實驗表明該探針能夠輕易地穿過細胞膜并靶向聚集于線粒體中,對線粒體內粘度進行熒光成像檢測。另外,通過EPR電子順磁共振儀檢測到Ir1Ir2在光照下能夠產生大量的單線態氧;同時發現配合物在腫瘤細胞中也能夠產生高毒性的單線態氧,使Ir1Ir2對A549細胞和Hep-G2細胞表現出很強的光毒性從而導致細胞死亡。
納米多孔Ni、Ni3S2/Ni復合電極的制備及其電催化析氫性能
周琦, 歐陽德凱, 汪帆, 何金山, 黎新寶
2021, 37(3): 412-420  doi: 10.11862/CJIC.2021.045
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采用脫合金化和水熱合成的方法制備納米多孔Ni和納米多孔Ni3S2/Ni復合電極。通過N2吸附-脫附測試、XRD、SEM、TEM等方法表征電極的孔徑分布、物相和微觀結構。在1 mol·L-1的NaOH溶液中,運用線性掃描伏安(LSV)曲線、交流阻抗(EIS)譜圖、恒電流電解法等測試電極的電催化析氫性能。結果表明:在電流密度為50 mA·cm-2時,與納米多孔Ni相比,Ni3S2/Ni合金具有更低的析氫過電位以及更高的析氫活性,同時納米多孔Ni3S2/Ni復合電極具有更低表觀活化能和電子轉移阻抗,進一步明確了過渡金屬硫化物對電催化析氫性能的特殊貢獻。
以9-蒽醛為熒光基團的吡唑啉衍生物熒光探針對Fe3+和Cu2+的檢測
羅杰偉, 趙波, 張仕祿, 賈飛云, 劉軍
2021, 37(3): 421-430  doi: 10.11862/CJIC.2021.048
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以9-蒽醛為熒光基團,嗎啉環和吡唑環為識別基團,合成了一種新型熒光探針1,5-二苯基-3-(10-(嗎啉甲基)蒽-2-基)吡唑啉(PMAP),利用1H NMR、13C NMR和單晶衍射表征其結構,通過熒光發射光譜和紫外可見吸收光譜研究其離子識別性能。結果表明,探針PMAP對Fe3+、Cu2+具有良好的識別效果,熒光量子產率分別從0.14降到0.05和0.04,溶液顏色從淡黃色變為藍色。PMAP與Fe3+/Cu2+以1:1的化學計量比形成配合物,檢測限約為1 μmol·L-1。同時,干擾實驗表明PMAP具有良好的抗干擾性能。在實際樣品中的應用表明,PMAP傳感器能有效地檢測實際水樣中的Cu2+和Fe3+。另外,根據Fe3+、Cu2+和H+不同組合時PMAP的量子產率構建了分子水平上的三輸入NOR邏輯門電路。
類姜黃素-芳基釕配合物的合成、結構和光照激活抗癌活性
蔣憲濤, 王曉輝, 李培源, 蘇煒
2021, 37(3): 431-436  doi: 10.11862/CJIC.2021.047
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合成了3種含姜黃素衍生物(L1~L3)和1,3,5-三氮雜-7-磷金剛烷(PTA)配體的芳基釕配合物[(η6-p-cymene)Ru(L)(PTA)]PF61~3,L=L1~L3),通過X射線單晶衍射、核磁共振波譜、高分辨質譜、元素分析等方法表征了這些配合物的結構,并用MTT法研究了它們在λ>400 nm的光照輔助下對HepG2人肝癌細胞的增殖抑制活性。結果表明,這3個配合物均為半三明治型結構;光輔助下,配合物抗癌活性明顯提高,其中配合物3對HepG2細胞的IC50值從(60.3±1.1)μmol·L-1降低至(45.0±6.1)μmol·L-1。說明光照可以有效提高此類配合物的抗腫瘤活性。
花球狀Bi2S3/BiOI復合光催化劑去除空氣中甲醛的應用
朱鳴凡, 盧澤強, 廖春鑫, 陳愛平, 李春忠
2021, 37(3): 437-442  doi: 10.11862/CJIC.2021.030
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以硫代乙酰胺為硫源,采用水熱陰離子轉移法,制備由納米片組裝的花球狀Bi2S3/BiOI復合光催化劑。以氣相甲醛作為模型污染物,在檢測艙中考察了復合催化劑對甲醛的去除作用。結果表明,具有異質結結構的Bi2S3/BiOI復合光催化劑具有較高的光催化活性,能在可見光下去除空氣中的甲醛,并且具有良好的循環使用穩定性。
Eu2+摻雜KCaCl3晶體的生長及發光性能
李嫚, 耿巨峰, 王昊宇, 楊晨樂, 潘尚可, 潘建國
2021, 37(3): 443-447  doi: 10.11862/CJIC.2021.049
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通過坩堝下降法生長出不同物質的量分數Eu2+摻雜的KCa1-xEuxCl3x=0.005、0.01、0.02、0.03、0.05)單晶,并對晶體進行了X射線粉末衍射、熱重、透過率、光致發光光譜、衰減時間、X射線激發發射光譜等測定。通過相圖及結構分析,判斷出該晶體為一致熔融化合物,并得出其為正交結構,晶胞參數為a=0.756 04 nm,b=1.048 23 nm,c=0.726 57 nm,空間群為Pnma(62)。在紫外光的激發下,晶體在434 nm左右有一個寬的發射峰,對應于Eu2+的4f65d1→4f7躍遷;光致衰減時間1.473 μs,晶體在X射線激發下的發光強度隨Eu2+離子濃度增加而增強。
ZrCdOx/SAPO-18雙功能催化劑催化CO2加氫合成低碳烯烴性能
楊浪浪, 孟凡會, 張鵬, 梁曉彤, 李忠
2021, 37(3): 448-456  doi: 10.11862/CJIC.2021.067
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采用并流共沉淀法制備了不同Zr/Cd原子比(nZr/nCd)的ZrCdOx金屬氧化物,并與水熱法制備的不同硅鋁比(nSiO2/nAl2O3)的片狀SAPO-18分子篩物理混合制得ZrCdOx/SAPO-18雙功能催化劑,研究了其催化CO2加氫直接合成低碳烯烴性能。采用透射電子顯微鏡(TEM)、X射線衍射(XRD)、N2吸附-脫附、CO2程序升溫脫附(CO2-TPD)、NH3程序升溫脫附(NH3-TPD)和X射線光電子能譜(XPS)對催化劑進行了分析。與單一ZrO2相比,引入CdO使得ZrCdOx比表面積下降,當nZr/nCd=8時制備的Zr8Cd1氧化物呈現出無定形小顆粒狀,Zr與Cd之間較強的協同作用使得ZrCdOx氧化物產生了更多的氧空位,有利于CO2的吸附活化。通過對Zr 8Cd1金屬氧化物與SAPO-18(硅鋁比0.1)的質量比、工藝反應溫度、壓力和空速對催化性能影響的考察,獲得了最佳反應條件。研究還發現,當SAPO-18的硅鋁比從0.1降為0.01時,Br?nsted酸含量降低,產物中烯烴/烷烴物質的量之比從18.6提高至37.2,但副產物CO含量迅速增加,低碳烯烴時空收率明顯下降。
氮摻雜泡沫碳電催化劑的制備及氧還原性能
李婧晗, 宋亞乘, 周亞洲, 程曉農, 楊娟
2021, 37(3): 457-464  doi: 10.11862/CJIC.2021.029
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利用水解乙烯基咪唑鎓硝酸鹽([Hvim]NO3)作為發泡劑和一次氮源,在碳化過程中實現材料自發泡。創造性地引入二次氮源三聚氰胺(C3H6N6),通過調控一次、二次氮源比例和碳化溫度,制備得到氮摻雜泡沫碳材料(HxMy-T,其中xy為一次和二次氮源的質量比,T對應不同的碳化溫度)。該方法提升了催化劑的氮摻雜含量,構建了更多有利于氧還原反應(ORR)的活性氮位點。電鏡結果顯示,催化劑H1M1-1000呈現出典型的泡沫碳孔洞結構和豐富的層狀褶皺結構;X射線光電子能譜測試結果表明,該樣品具有較高的活性氮含量(原子分數6.77%),吡啶氮和石墨氮的原子分數分別高達22.23%和55.59%;電化學測試結果表明,該樣品在堿性環境中的半波電位為0.834 V(vs RHE),與商業Pt/C相當,且具有優于商業Pt/C的抗甲醇性能和穩定性。
基于苯四甲酸和雙(咪唑基甲基)苯配體的三維Cd-MOF的合成、結構及熒光性質
楊華, 吳雨澤, 崔華莉, 劉琳, 王記江, 陳小莉
2021, 37(3): 465-472  doi: 10.11862/CJIC.2021.051
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選擇剛性的1,2,4,5-均苯四甲酸(H4L)為主配體,以1,3-雙(1H-咪唑-1-基甲基)苯(1,3-bib)為輔助配體,在水熱條件下,與過渡金屬離子Cd2+配位合成了配合物[Cd(L)0.5(1,3-bib)(H2O)]·H2O(1)。利用元素分析、紅外光譜、X射線單晶衍射、熱重和X射線粉末衍射對其結構進行了表征,并研究了化合物的熒光性質。結果表明:配合物1屬正交晶系,空間群Pbca,a=0.857 08(4)nm,b=1.912 23(10)nm,c=2.451 60(12)nm。配合物1中Cd2+與L4-配體的羧基通過雙齒螯合配位,通過1,3-bib連接形成三維網狀結構。配合物1具有較強的熒光,其對丙酮溶劑、MnO4-、Hg2+離子有一定的熒光猝滅。
三維多孔碳負載氧化錫并協同氟化鋰制備高性能鋰離子陽極
何強, 孫曉剛, 鄒婧怡, 李銳
2021, 37(3): 473-481  doi: 10.11862/CJIC.2021.059
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新型多孔碳納米片/碳納米管(PC/CNT)材料表現出豐富的分級孔隙結構,具有較高的氧化錫(SnO2)負載量。通過PC和CNT交聯形成的三維結構能夠有效地提高鋰離子傳輸速率和電子的傳導。此外,在電極中摻雜的氟化鋰(LiF)不僅能夠降低SnO2-PC/CNT-LiF電極的電荷轉移電阻,而且還能補充SEI膜形成時消耗的Li+,降低不可逆容量,增強SEI膜的穩定性。研究表明,SnO2-PC/CNT-LiF電極在電流密度為100 mA·g-1時,首次可逆比容量達到1 642.98 mAh·g-1,活性物質的利用率高達90.12%,循環100次后,放電比容量仍然達到745.11 mAh·g-1,且庫侖效率仍然保持在95.1%以上,顯示出優異的倍率和循環性能。
Ag/MgO串聯協同催化降解偶氮染料
祝曉輝, 郭紫薇, 劉向東, 李仁宏, 韋童
2021, 37(3): 482-490  doi: 10.11862/CJIC.2021.058
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以納米氧化鎂為載體,采用浸漬法制備一系列過渡金屬負載型催化劑。測試其對染料的降解性能后篩選出了效果最優的催化劑Ag/MgO,并采用X射線衍射(XRD)、X射線光電子能譜(XPS)、透射電子顯微鏡(TEM)、擴展X射線吸收精細結構譜(EXAFS)以及X射線吸收近邊結構(XANES)等表征方法對該催化材料的結構特征、微觀形貌進行分析。通過表征分析發現Ag是以納米簇的形式均勻地分散在MgO表面,Ag和Mg之間形成了雙金屬位點,且催化劑中Ag的電子密度較高,從而具有較高的催化活性。在甲醛溶液中,在室溫、無需光熱等條件下即可高效降解偶氮染料AR1。該反應體系中影響降解效果的因素主要是溫度和甲醛濃度,溫度升高,降解效率增大,但甲醛濃度有最優值(1 mol·L-1)。通過自由基捕獲實驗測得反應中有2種自由基在發揮作用,即具有還原性的氫自由基和具有氧化性的超氧自由基,它們的協同作用可以將染料分子中的顯色基團(-N=N-)輕易地破壞,這種“還原-氧化”的協同作用機制提高了反應效率。此外,醛類也是常見污染物之一,將其作為助劑的同時達到了“以污治污”的效果。
靜電紡絲法制備納米氧化銦錫及其導電性能
任鑫川, 劉蘇婷, 李志慧, 宋承堃, 代云茜, 孫岳明
2021, 37(3): 491-498  doi: 10.11862/CJIC.2021.020
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采用靜電紡絲-溶膠凝膠法,以SnCl2、InCl3、聚乙烯吡咯烷酮(PVP)等為原料,乙醇胺為水解控制劑,合成了超細氧化銦錫(ITO)納米纖維及富氧缺陷的ITO納米顆粒。采用透射電子顯微鏡(TEM)、選區電子衍射(SAED)、掃描電子顯微鏡(SEM)、熱重分析(TGA)、X射線衍射(XRD)、X射線電子能譜(XPS)、四探針電阻儀,系統研究了超細ITO纖維及顆粒的形貌、晶型、氧缺陷及導電性能。在400℃空氣煅燒后,纖維中的PVP高分子骨架發生熱分解,獲得超細、多孔ITO納米纖維,晶型為立方相。進一步升高煅燒溫度至800℃,ITO納米纖維轉變為富氧缺陷的納米顆粒,晶格氧空位含量高達38.9%。隨著煅燒溫度升高,Sn4+摻入到In2O3晶格中,發生晶格膨脹,晶面間距增大。煅燒溫度由400℃升高至800℃,未發生立方相向六方相的轉變,晶型穩定,晶粒尺寸從32 nm生長到44 nm,晶格應變(ε0)從1.943×10-3減小至1.422×10-3,應變誘導的晶格弛豫逐漸減小。此外,高溫煅燒可抑制In2O3晶粒(111)晶面的增長,隨著In2O3的(400)與(222)晶面比值(I(400)/I(222))的增加,ITO電導率逐漸升高。在800℃獲得的ITO納米顆粒導電率最高。
兩步電沉積構建NiFe/Ni3S2/NF分級異質電極用于大電流密度析氧反應
張議潔, 劉樂然, 武昀, 趙斐, 劉光, 李晉平
2021, 37(3): 499-508  doi: 10.11862/CJIC.2021.057
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通過簡便的兩步電沉積法在泡沫鎳表面有效復合非晶態Ni3S2材料與富缺陷的NiFe雙金屬羥基氧化物,從而構建了NiFe/Ni3S2/NF三維分級納米異質電極。受益于非晶態Ni3S2和富缺陷NiFe材料的結構和催化優勢,以及異質界面的強電子相互作用,使得NiFe/Ni3S2/NF催化電極表現出優異的析氧催化性能:達到100 mA·cm-2時的析氧過電位僅為273 mV,遠優于大多數已報道的Ni/Fe基復合材料。值得注意的是,在1 mol·L-1 KOH溶液中,僅需~372 mV的過電位即可穩定輸出1 000 mA·cm-2的高電流密度達27 h以上。
p區金屬氧化物Ga2O3和Sb2O3光催化降解鹽酸四環素性能差異
毛婧蕓, 黃毅瑋, 黃祝泉, 劉欣萍, 薛琿, 肖荔人
2021, 37(3): 509-515  doi: 10.11862/CJIC.2021.063
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摘要:
對沉淀法合成的p區金屬氧化物Ga2O3和Sb2O3紫外光光催化降解鹽酸四環素的性能進行了研究,討論了制備條件對光催化性能的影響。最佳制備條件下得到的Ga2O3-900和Sb2O3-500樣品光催化性能存在巨大差異,通過X射線粉末衍射、傅里葉紅外光譜、N2吸附-脫附測試、熒光光譜、拉曼光譜、電化學分析及活性物種捕獲實驗等對樣品進行分析,研究二者光催化降解鹽酸四環素的機理,揭示影響光催化性能差異的本質因素。結果表明,Ga2O3和Sb2O3光催化性能差異主要歸結于二者不同的電子和晶體結構、表面所含羥基數量及光催化降解機理。
Articles
Preparation and Fluorescent Properties of LiBa0.95-yBO3: 0.05Tb3+, yBi3+
Ya LU, Min-Zhi ZHANG, Gang-Feng LIANG, Chun-Xia LI, Guo-Liang ZHAO
2021, 37(3): 516-524  doi: 10.11862/CJIC.2021.066
[摘要]  (19) [HTML全文] (19) [PDF 13716KB] (0)
摘要:
Two series of phosphors of Tb3+ single doped LiBa1-xBO3: xTb3+ (molar fraction x=0.02, 0.03, 0.04, 0.05, 0.06, 0.07) and Bi3+/Tb3+ co-doped LiBa0.95-yBO3: 0.05Tb3+, yBi3+ (molar fraction y=0.02, 0.03, 0.04, 0.05, 0.06, 0.07) of which can be effectively excited by (near) ultraviolet at 369, 254 nm light were prepared by high temperature solid state reaction from boric acid and carbonates. The structures and morphology of the samples were characterized by powder X-ray diffraction (PXRD) and scanning electron microscopy. PXRD measurement shows that the products of the two series are pure phase LiBaBO3. By measuring the fluorescent spectra of the first series of products, the product with the best luminescent intensity was screened out, and the optimal doping amount of Tb3+ was determined accordingly; on this basis, the second series of phosphors with different doping amounts of Bi3+ were prepared. The experimental results of fluorescent spectra show that the luminescent intensity of Tb3+/Bi3+ co doped phosphors was better than that of Tb3+ single-doped phosphors, indicating that Bi3+ sensitizes to Tb3+; the fluorescent intensity of the products increased first and then decreased with the increase of Bi3+ content, and the luminescence intensity of the products reached the maximum when the doped molar fraction y of Bi3+ was 0.03. The energy transfer from Bi3+ to Tb3+ ions is attributed to the dipole quadrupole interaction. The CIE chromaticity coordinates of the phosphors show that the luminescent color exhibited a gradual trend from green to white in some degree.
Synthesis and Magnetic Characterization of Mononuclear Co(Ⅱ) Complex Based on Pyrazine-Containing Hydrazone Schiff Base Ligand
Yu CHEN, Zhao-Dong WANG
2021, 37(3): 525-530  doi: 10.11862/CJIC.2021.050
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摘要:
A mononuclear Co(Ⅱ)complex (NHEt3)[Co(HL)2] ·3H2O (1) based on a pyrazine-containing hydrazone Schiff base ligand H2L was synthesized and characterized by IR, thermogravimetric analysis, X-ray single diffraction and magnetic susceptibility measurements. X-ray single crystal analysis reveals that it consists of a Co(Ⅱ)ion, two deprotonated HL- ligands, three uncoordinated H2O and a protonated triethylamine. The central Co(Ⅱ)ion is six- coordinated with N2O4 donor sets to form distorted octahedral geometry. Magnetic susceptibility measurement of both complex 1 and the dehydrated 1 showed a gradual high spin to low spin transition, and the differences can be attributed to the hydrogen bonding effects on the magnetic properties. CCDC: 1973542, 1 (298 K); 20274281, 1 (100 K).
Preparation and Photocatalytic Activity of Ag/Ag2MoO4/Bi2MoO6 Composite Photocatalyst
Shuai-Shuai MA, Cheng-Juan HUANG, Yu-Qing ZONG, Jian-Dong GU, Zhao-Lian YE, Jin-Juan XUE
2021, 37(3): 531-540  doi: 10.11862/CJIC.2021.055
[摘要]  (19) [HTML全文] (19) [PDF 7050KB] (0)
摘要:
A novel Ag/Ag2MoO4/Bi2MoO6 ternary photocatalyst was successfully prepared by hydrothermal, chemical deposition and in-situ photoreduction process. The as-prepared photocatalysts were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS) and UV-visible diffuse reflection spectroscopy (UV-Vis DRS) to investigate the composition, morphology, optical absorption characteristics and photoelectrochemical properties. The photocatalytic performance of Ag/Ag2MoO4/Bi2MoO6 photocatalyst was evaluated with tetracycline as the target pollutant under visible light. The research results show that, compared with pure Ag2MoO4 and Bi2MoO6, the surface plasmon resonance (SPR) effect of Ag significantly broadens the visible light absorption capacity and response range of the catalytic system. When the theoretical loading (mass fraction) of Ag2MoO4 was 24.6%, Ag/Ag2MoO4/Bi2MoO6 ternary photocatalyst could completely degrade tetracycline within 20 min, and maintained high catalytic activity after 5 cycles of use, showing good cycle stability.
Enhancement of Visible-Light Catalytic Activity for Zn Doped OV-β-Bi2O3: Regulation of Electronic Structure and Promotion of Charge Separation
Ya-Wen ZHAO, Jun-Ke ZHANG, Cai-Xia FENG, Jia-Peng XU, Rui DU, Hua HU, Yan-Mei ZHOU, Shan-Hu LIU, Yan-Hong LIU
2021, 37(3): 541-554  doi: 10.11862/CJIC.2021.064
[摘要]  (17) [HTML全文] (17) [PDF 14304KB] (1)
摘要:
A novel Zn-doped β-Bi2O3 nanomaterial (OV-Zn: Bi2O3) with two crystal defects, oxygen vacancy (OV) and doped Zn2+, was prepared via a sol-gel method followed by in-situ carbon thermal reduction treatment. The concentration of OV of OV-Zn: Bi2O3 sample can be modulated by regulating the content of doped Zn2+. As a reference, the novel β-Bi2O3 having OV but without doped Zn2+ (OV-β-Bi2O3) was also synthesized via a similar process. The comprehensive effect of OV and doped Zn2+ on the visible-light-activity of OV-Zn: Bi2O3 for the degradation of methylene blue (MB) and 2, 4, 6-trichlorophenol (2, 4, 6-TCP) was investigated by ultraviolet-visible light diffuse reflectance spectra, X-ray photoelectron spectra, electron spin resonance, photoluminescence spectrum and photoelectrochemical measurements. The results show that introduction of OV can not only drastically extend the photoabsorption into longer wavelength region but also promote the separation of photo-generated charge carriers. So, compared to traditional β-Bi2O3, OV-β-Bi2O3 demonstrated highly promoted activity for the degradation of methylene blue (MB) and 2, 4, 6-trichlorophenol (2, 4, 6-TCP). For OV-Zn: Bi2O3 catalysts, Znic doping can make the valence band edge of catalysts move down and the oxidation ability of photo-excited holes increase. And appropriate amount of zinc doping can also improve the separation efficiency of photogenerated carriers. In contrast to OV-β-Bi2O3, the visible light activity of OV-Zn: Bi2O3 was further improved and OV-Zn: Bi2O3-0.3 with a molar ratio (nZn/nBi) of 0.3 exhibited the highest activity for the degradation of MB and 2, 4, 6-TCP.
Y-Mn-O Supported Ni-Based Catalyst for Hydrogen Production via Auto-thermal Reforming of Acetic Acid
Xiao-Min HU, Hui CHEN, Xuan-Yi JIA, Qiao WANG, Li-Hong HUANG
2021, 37(3): 555-560  doi: 10.11862/CJIC.2021.032
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摘要:
To effectively achieve high hydrogen yield from biomass-derived acetic acid (HAc), a series of NiMnY catalysts were prepared by hydrothermal method and tested in auto-thermal reforming (ATR) of HAc. X-ray diffraction (XRD), N2 adsorption-desorption test and H2-temperature-programmed reduction (H2-TPR) were carried out to explore the internal relationship within these NiMnY catalysts. Over the Ni0.39Mn0.61YO3.11±δ catalyst, perovskite-like (Ni, Mn)YO3 phase was formed after calcination, and converted into thermostable Ni-Mn-Y-O species after reduction in H 2, along with the highly dispersed nickel nanoparticles. As a result, over the promoted Ni0.39Mn0.61YO3.11±δ catalyst, a stable catalytic performance with high HAc conversion (100%) and hydrogen yield (2.68 molH2 ·molHAc-1) was recorded, showing potential for hydrogen production.
Syntheses and Crystal Structures of Two Copper Complexes Based on Thienyl and Pyridyl Substituted Triaryltriazoles
Gang LI, Zhe FENG, Rong-Rong NIE, Dun-Ru ZHU
2021, 37(3): 561-568  doi: 10.11862/CJIC.2021.054
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摘要:
Two new copper(Ⅱ) complexes, trans-[Cu(L1)2(MeOH)2](ClO4)2 (1) and trans-[Cu(L2)2(ClO4)2]·2MeCN (2) (L1=3-(2-pyridyl)-4-phenyl-5-(2-thienyl)-1, 2, 4-triazole, L2=3-(2-pyridyl)-4-(p-chlorophenyl)-5-(2-thienyl)-1, 2, 4triazole), were synthesized and structurally characterized by FT-IR, elemental analyses, single-crystal X-ray crystallography and powder X-ray diffraction. Both 1 and 2 crystallize in monoclinic system with a space group P21/c. Xray crystallography analysis reveals that the copper ion in 1 and 2 sits in a distorted octahedral environment[CuN4O2] with two MeOH in the trans-position in 1 but two ClO4- in the trans-position in 2. Each L ligand in the equatorial plane adopts a chelating bidentate mode through the pyridyl N atom and one triazole N atom, while the thienyl group does not coordinate. 2 contains two MeCN guest molecules which produce π-π stacking interactions with the triazole ring. In 1 and 2 there are some intermolecular O-H…O, C-H…O and C-H…N hydrogen bonds and C-H…π interactions, linking the mononuclear complexes to form a 3D framework. CCDC: 2423470, 1; 2423471, 2.
Theoretical Study on Regulation of Aniline Moiety on Non-radiative Transition of a Kind of Pt(Ⅱ) Phosphorescent Materials
Guo-Jun KANG, Ke LI, Xue-Feng REN, Hong-Qu TANG
2021, 37(3): 569-576  doi: 10.11862/CJIC.2021.065
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摘要:
A series of efficient red platinum based emitter with functionalized diphenylamine moiety (M1~M3) were designed and investigated by density functional theory (DFT) and time-dependent DFT (TD-DFT). The effect of different substituent positions on the electronic structures and optical properties were fully explored by compared with the synthesized complex. The introduction of diphenylamine moiety could effectively strengthen the π-conjugation interaction between the metal and ligand. By gradually increasing the amount of diphenylamine moiety, the intensities and the participation of metal-to-ligand charge-transfer (MLCT) for the absorption bands of M3 were enhanced, which are beneficial to collect light energy participation of metals and increase the spin-orbital coupling effect. M1~M3 exhibited red emission with the peak wavelengths at 602~630 nm. These emission spectra are mixtures of 3MLCT and ligand to ligand charge transfer (3LLCT) character. The possible non radiative process T1 (3MLCT) → TS → triplet metal-centered 3MC (d-d) state were deeply investigated, and the results show that the possibility of the non-radiative process will decrease because the surface crossing at a minimum energy crossing point (MECP) between T1 and S0 state is difficult to populate when the functionalized diphenylamine moiety is useful to enhance steric hindrance.
綜述
鉍基納米材料在癌癥成像診斷與治療中的應用
劉應兵, 于文生, 王進賢, 董相廷, 付振東, 劉桂霞
2021, 37(1): 1-15  doi: 10.11862/CJIC.2021.013
[摘要]  (99) [HTML全文] (99) [PDF 44132KB] (99)
摘要:
隨著納米醫學的快速發展,納米診療材料因其兼具診斷和治療等多功能性而受到越來越多的關注。鉍(Bi)基納米材料具有優異的光學、電學和磁學性質,在腫瘤的診療一體化領域具有廣闊的應用前景。我們總結了Bi基納米材料常用的構建方法,重點介紹了其在計算機斷層掃描(CT)成像、光聲(PA)成像、放射療法(RT)、光熱療法(PTT)及協同作用方面的應用研究進展,并對其未來發展進行了總結和展望。
論文
混合熔鹽法低溫合成Sm2Ti2S2O5及其光催化分解水產氫
晁明坤, 馬貴軍
2021, 37(1): 16-22  doi: 10.11862/CJIC.2021.006
[摘要]  (83) [HTML全文] (83) [PDF 6750KB] (83)
摘要:
以TiO2、TiS2及Sm2O3為前驅體,分別加入LiCl-KCl與LiCl-CsCl的最低共熔混合物作為熔鹽,在較低溫度下成功合成了Sm2Ti2S2O5(STSO)顆粒。通過對比不同溫度下所制備產物的X射線衍射圖,首次表明STSO的熱力學結晶溫度在520℃左右,遠低于之前報道的650℃的最低合成溫度。掃描電子顯微鏡照片顯示,采用2種混合熔鹽制備的STSO都呈片狀形貌;同一合成溫度下,采用LiCl-CsCl熔鹽制備的STSO的厚度小于LiCl-KCl所得產物。采用出射光波長大于420 nm的氙燈作為光源,在含有Na2S-Na2SO3空穴犧牲劑的溶液中,所制備的STSO顆粒表現出最高35 μmol·h-1的光催化分解水產氫活性以及20 h以上的產氫穩定性。
鹽酸氯丙嗪對八肋游仆蟲中心蛋白C端功能的抑制
董倩, 葉旭文, 楊靜, 王文明, 趙亞琴, 楊斌盛
2021, 37(1): 23-32  doi: 10.11862/CJIC.2021.019
[摘要]  (76) [HTML全文] (76) [PDF 7248KB] (76)
摘要:
通過熒光光譜分析、等溫滴定量熱(ITC)、圓二色譜(CD)、電泳等技術研究了鹽酸氯丙嗪(CPZ)和八肋游仆蟲中心蛋白C端(apoC-EoCen)的結合以及CPZ對蛋白功能的影響。結果表明,在室溫下10 mmol·L-1 Hepes溶液(pH=7.4)中,CPZ與apoC-EoCen以物質的量之比為1:1結合,條件結合常數約為104L·mol-1。CPZ的結合導致蛋白質的二級結構發生改變,α螺旋含量減??;對金屬離子誘導中心蛋白的聚集產生了抑制作用,Tb3+敏化熒光強度也降低;阻礙了中心蛋白與著色性病干皮病C組蛋白(XPC)的結合;且影響了apoC-EoCen類核酸酶活性,導致蛋白對pBR322 DNA的切割能力下降;抑制了蛋白質的磷酸化。綜合實驗結果表明鹽酸氯丙嗪是中心蛋白的生物功能阻斷劑,對中心蛋白的功能具有良好的調控作用。
以2-(2-吡啶基)苯并噻吩為主配體的兩種藍紫光二價鉑配合物的合成與性質
王登強, 陳宇, 劉小慶, 卞健健, 尹新穎, 滕明瑜, 戎梅竹, 汪正良
2021, 37(1): 33-38  doi: 10.11862/CJIC.2021.012
[摘要]  (79) [HTML全文] (79) [PDF 1954KB] (79)
摘要:
以2-(2-吡啶基)苯并噻吩(2-(2-pyridyl)benzothiophene,btp)作為主配體,分別以鄰二氮菲[1, 10]并咪唑聯苯酚(2-(1H-imidazo[4,5-f][1, 10]phenanthrolin-2-yl)phenol,ipap)和3-甲基-6-苯基咪唑[2,1-b]噻唑(3-Methyl-6-phenylimidazo[2,1-b]thiazole,mpmt)作為輔助配體,成功合成了2個二價鉑配合物[(btp)Pt(ipap)]Cl與(btp)Pt(mpmt)Cl,并得到了配合物(btp)Pt(mpmt)Cl的晶體結構。由金屬-配體電荷轉移引起的2種配合物發光,具有60%左右的內量子效率,發射峰在426 nm(藍色)與381 nm(紫色)處。HOMO/LUMO軌道能級分別為-4.69 eV/-2.55 eV與-4.80 eV/-2.21 eV。單晶衍射結果表明,較低的共軛程度導致了該類配合物的短波長發射。
溶膠-凝膠法制備Fe摻雜MgF2催化劑及其催化1,1-二氟乙烷(R152a)脫HF反應的性能
張蕾, 李雨臻, 李利春, 韓文鋒, 李瑛, 唐浩東
2021, 37(1): 39-46  doi: 10.11862/CJIC.2021.021
[摘要]  (75) [HTML全文] (75) [PDF 10307KB] (75)
摘要:
通過助劑摻雜的方法解決MgF2催化劑高溫失活的問題。采用溶膠-凝膠法制備了一系列Fe3+摻雜的高比表面MgF2催化劑,并通過N2吸附-脫附測試、X射線衍射(XRD)、能量色散X射線光譜(EDS)和NH3程序升溫脫附技術(NH3-TPD)、電子自旋共振(ESR)、X射線光電子能譜(XPS)等對FeF3/MgF2催化劑的物化性質進行了表征。結果表明,一定量(物質的量分數小于20%)的Fe3+摻雜可以有效地減少MgF2晶粒度,且隨著Fe3+摻雜量的增加,催化劑的比表面積、酸性及1,1-二氟乙烷(R152a,C2H4F2)脫HF反應的催化活性均呈現增加趨勢,但當Fe3+摻雜量超過20%時,催化劑明顯失活。
三維α-MnO2@Co3O4異質材料的制備、表征及其催化性能
劉恒發, 謝鈺, 劉琪, 程高, 孫明, 余林
2021, 37(1): 47-54  doi: 10.11862/CJIC.2021.003
[摘要]  (79) [HTML全文] (79) [PDF 17321KB] (79)
摘要:
α-MnO2納米線為基底,原位生長ZIF-67,再經焙燒轉化為三維α-MnO2@Co3O4異質材料,并用于甲苯的催化燃燒反應。結果表明:粒徑大小約為12 nm的Co3O4納米顆粒均勻生長在MnO2納米線外表面,形成異質界面。該復合材料的低溫可還原性能更佳,具有更多的表面活性氧物種。相比于α-MnO2納米線,α-MnO2@Co3O4表現出更佳的甲苯催化燃燒性能:起燃溫度(轉化率10%)T10為202℃,完全燃燒溫度(轉化率90%)T90為235℃。
復合催化劑α-(Fe,Cu)OOH/RGO的制備、表征及其協同H2O2在可見光下去除環丙沙星性能
許俊鴿, 洪俊賢, 胡蝶
2021, 37(1): 55-64  doi: 10.11862/CJIC.2021.008
[摘要]  (93) [HTML全文] (93) [PDF 7674KB] (93)
摘要:
采用一步回流法制備了α-(Fe,Cu)OOH/RGO復合催化劑,通過粉末X射線衍射、掃描電子顯微鏡和X射線光電子能譜等對催化劑進行了表征,并以30 mg·L-1的環丙沙星(CIP)為目標污染物,研究了不同制備條件下所得催化劑在可見光照射下協同H2O2對CIP的去除效果。結果表明,成功實現了α-(Fe,Cu)OOH納米棒在石墨烯二維薄片上原位生長,α-(Fe,Cu)OOH/RGO復合材料的可見光吸收邊發生紅移,禁帶寬度從2.02 eV變為1.76 eV。石墨烯復合不但增強了對污染物的吸附能力,而且加快了光生電子的分離、遷移速率,還提高了反應體系中電子的傳導效率。當石墨烯復合比例(質量分數)為1%時,復合催化劑的催化性能最佳。當催化劑投加量為0.40 g·L-1,H2O2濃度為0.10 mol·L-1時,反應120 min,CIP被全部去除。α-(Fe,Cu)OOH/RGO循環使用5次,對CIP的去除率均在90%以上,表明催化劑具有較強的催化活性和較好的穩定性。
巰基/羧基修飾硅藻土及其對Pb(Ⅱ)、Cd(Ⅱ)的吸附性能
杜玉成, 李生輝, 谷恒學, 李楊, 吳俊書, 靳翠鑫
2021, 37(1): 65-73  doi: 10.11862/CJIC.2021.025
[摘要]  (83) [HTML全文] (83) [PDF 20944KB] (83)
摘要:
以3-巰基丙基三甲氧基硅烷(MPTS)、3-氨基丙基三乙氧基硅烷(APTES)、檸檬酸(CA)為原料,采用水浴法、水浴/低溫水熱法,分別制備了巰基(—SH)、氨基/羧基(—NH2/—COOH)表面修飾的硅藻土。采用傅里葉變換紅外光譜、掃描電子顯微鏡、氮氣吸附-脫附測試、熱重/差示掃描量熱法、X射線光電子能譜等技術對樣品進行了表征,并探討分析了樣品制備機理。當重金屬離子溶液pH=7,吸附時間為4 h時,以MPTS制備的巰基修飾硅藻土吸附劑對Pb(Ⅱ)、Cd(Ⅱ)的最大吸附容量分別為396、365 mg·g-1;以APTES、CA制備的氨基/羧基縮合修飾硅藻土吸附劑對Pb(Ⅱ)、Cd(Ⅱ)最大吸附容量分別為485、462 mg·g-1。
三元混配銅(Ⅱ)配合物的晶體結構、DNA作用及其生物活性
蔡戴宏, 莫慧雯, 何良, 樂學義
2021, 37(1): 74-84  doi: 10.11862/CJIC.2021.026
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摘要:
利用溶劑緩慢揮發法合成了以5-氯-2-(2'-吡啶基)苯并咪唑為主配體、L-苯丙氨酸根為輔助配體的三元混配銅(Ⅱ)配合物:[Cu(HPBC)(L-Phe)(H2O)]ClO4(簡稱為1,HPBC=5-氯-2-(2'-吡啶基)苯并咪唑,L-Phe=L-苯丙氨酸根)。采用元素分析、紅外光譜、紫外可見光譜、摩爾電導率測定和電噴霧質譜等手段對配合物1進行了表征,利用X射線單晶衍射確定配合物具有五配位的變形四方錐構型,并通過電子吸收光譜、熒光光譜、粘度測定及分子對接等方法揭示了配合物主要以插入作用的方式與小牛胸腺DNA(CT-DNA)結合。配合物對被測微生物(李斯特菌、金黃色葡萄球菌和大腸桿菌)及癌細胞(SGC-7901、Bel-7402、HeLa和A549)顯示出良好的抗菌和細胞毒活性(IC50=1.69~2.50 μmol·L-1)。最重要的是,通過確定細胞的形態變化(AO/EB雙染法)及細胞周期測定分析,揭示了配合物1通過DNA結合的途徑誘導SGC-7901細胞凋亡。
基于1D/0D有序復合SnO2納米晶的鈣鈦礦太陽能電池
劉德政, 楊高元, 向文灝, 王松, 李望南, 鐘杰, 黃福志, 陳美華, 梁桂杰
2021, 37(1): 85-94  doi: 10.11862/CJIC.2021.005
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摘要:
通過水熱前驅體中的功能添加劑調控一維(1D)納米棒陣列疏密度,繼而在納米棒間隙沉積零維(0D)納米顆粒,制備1D/0D有序的復合SnO2電子傳輸層(ETL),并組裝高效、穩定的鈣鈦礦太陽能電池。系統研究前驅體中NaCl添加劑以及后續納米顆粒的沉積對復合ETL的形貌結構、光譜性能及界面電荷過程的作用規律,探討上述作用對電池光電性能的影響機制。前驅體中NaCl的加入使棒密度變小,從而使0D納米顆粒順利滲透到1D納米棒間隙中,其對鈣鈦礦/ETL和鈣鈦礦/FTO界面復合的抑制作用是造成器件開路電壓和填充因子增大的原因。在經2 mL飽和NaCl水溶液改性的1D電子傳輸層ETL-2Cl的基礎上,繼續沉積0D的納米顆粒,制備得到新型1D/0D復合電子傳輸層ETL-2P,后者優良的電荷復合抑制作用(復合電阻是ETL-2Cl的2.9倍)和高效的電子抽提性能(抽提速率3.03×107 s-1,抽提效率91.6%)促成了電池較優的光電性能(光電效率12.15%)。
Mn、Mg共摻雜Ni(OH)2的電化學性能
姚壽廣, 竇飛, 劉頓, 程杰
2021, 37(1): 95-102  doi: 10.11862/CJIC.2021.014
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摘要:
采用緩沖溶液法制備復合摻雜Mn、Mg的正極材料Ni0.82Mn0.18-xMgx(OH)2(x=0.06、0.09、0.12)。采用XRD、XPS和SEM等測試表征材料的晶體結構、錳價態和形貌,采用循環伏安和恒流充放電測試研究Mn、Mg不同摻雜比例對氫氧化鎳電化學性能的影響。結果表明,Mn、Mg摻雜樣品均為β相,晶粒細化;Ni0.82Mn0.09Mg0.09(OH)2樣品具有優異的電極反應可逆性和充放電性能,100 mA·g-1電流密度下的放電比容量(290.6 mAh·g-1)優于商用β-Ni(OH)2(281.1 mAh·g-1);且500 mA·g-1電流密度下循環30圈后,Ni0.82Mn0.09Mg0.09(OH)2的放電比容量未見衰減,其循環穩定性優于商用β-Ni(OH)2。
鉻-對苯二甲酸MOF的框架異構:MIL-88B(Cr)和MIL-101(Cr)
趙田, 朱和鑫, 董茗, 趙熠
2021, 37(1): 103-109  doi: 10.11862/CJIC.2021.018
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可以通過簡單地控制乙酸濃度的方法,在相似的水熱合成條件下合成2種同一家族的金屬有機框架材料(MOFs):MIL-88B(Cr)和MIL-101(Cr)。在相對較低的乙酸濃度下,可以得到平均粒徑為100 nm的MIL-101(Cr),并擁有很高的BET比表面積(3 543 m2·g-1)。而在相對較高的乙酸濃度下,則可得到另一種具有“呼吸”特性結構的MOF——MIL-88B(Cr)。利用粉末X射線衍射、掃描電鏡、N2吸附-脫附分析、熱重分析等對它們的結構、形貌、孔隙率等性質做了詳細的分析。
高鎳系正極材料LiNi0.88Co0.07Al0.05O2的制備及性能表征
羅京, 劉建雄, 黃玲, 肖方明, 李文超, 唐仁衡, 王英
2021, 37(1): 110-120  doi: 10.11862/CJIC.2021.010
[摘要]  (74) [HTML全文] (74) [PDF 46310KB] (74)
摘要:
以鎳鈷氫氧化物為原料,采用異丙醇鋁水解法合成Ni0.88Co0.07Al0.05(OH)2,將前驅體與鋰源充分混合,通過3種燒結條件制備出球形LiNi0.88Co0.07Al0.05O2正極材料,借助X射線衍射(XRD)、掃描電鏡(SEM)、透射電鏡(TEM)、X射線光電子能譜(XPS)以及電化學測試等表征手段對材料的晶體結構、微觀形貌和電化學性能進行了較系統的研究。研究表明,在500℃下保溫3 h、700℃下保溫14 h的條件下合成的LiNi0.88Co0.07Al0.05O2具有良好的綜合電化學性能,0.2C放電比容量達192.2 mAh·g-1,首次充放電效率為81.6%,1C放電比容量為190.7 mAh·g-1,100周后放電比容量為141.1 mAh·g-1,容量保持率達到73.4%。
Articles
Preparation, Structures and Thermal Stabilities of Four Transition Metal Complexes Constructed by 3, 7-Di(3-pyridyl)-1, 5-dioxa-3, 7-diazacyclooctane Bipyridine Ligand
Li LI
2021, 37(1): 121-130  doi: 10.11862/CJIC.2021.009
[摘要]  (63) [HTML全文] (63) [PDF 5547KB] (63)
摘要:
Four transition metal complexes, [Co(NO3) (H2O)2(L)2]NO3 (1), [Co2Cl4(L)2] ·CH2Cl2 (2), [Cd2(AcO)4(L)2] ·4CH3OH (3) and[Cd2(NO3)2(CH3OH)2(H2O)2(L)2](NO3)2·2H2O (4), were synthesized by employing a clamplike bipyridine ligand 3, 7-di(3-pyridyl)-1, 5-dioxa-3, 7-diazacyclooctane (L). Single-crystal X-ray analysis reveals that complex 1 is mononuclear structure; 2 is macrocyclic dimer; wheras 3 and 4 are rectangular dinuclear structures. The ligand molecules in these complexes has shown three types of coordination mode including mono-dentate, trans-bridge and cis-bridge. All of the complexes were also characterized by elemental analysis, IR, thermal stabilities and singlecrystal structure analysis.CCDC: 940778, 1; 915840, 2; 1446573, 3; 1446574, 4.
Reviews
Ni(OH)2 with Super-Small Nanoscale: Synthesis and Application in Li+ Adsorptions
Nan JING, An-Nan ZHOU, Guo-Hui WANG, Run-Wei WANG, Qing-Hong XU
2021, 37(1): 131-139  doi: 10.11862/CJIC.2021.015
[摘要]  (77) [HTML全文] (77) [PDF 13885KB] (77)
摘要:
α-Ni(OH)2 nanoparticles with 5 nm average diameter were prepared under the existence of glucose in water solution, and the size of α-Ni(OH)2 nanoparticles was found to be controlled by the concentration of glucose. A possible mechanism of the preparation process was proposed. When the synthesis was processed without existence of the glucose, β-Ni(OH)2 was obtained. The super-small α-Ni(OH)2 nanoparticles showed strong adsorption ability to Li+ ions when pH value of the solution was about 7.0 under room temperature. Maximum adsorption capacity of the super-small α-Ni(OH)2 nanoparticles to Li+ was about 214 mg·g-1; however, the β-Ni(OH)2 with diameter above 1.0 μm was low than 30 mg·g-1. Freundlich equation analysis and SEM images of the adsorption products indicate multilayers' adsorption process to Li+ of α-Ni(OH)2 nanoparticles.
Dynamic Formation of Pdδ+-Fe2+ Interface Promoting Reverse Water Gas Shift Reaction over Pd/FeOx Catalyst
Dian-Yu ZHANG, Fang LIU, Peng-Fei DU, Meng-Wei LI, Zhao-Xuan WU, Yi-Bing FENG, Yang ZHAO, Xiao-Yan XU, Xin-Xing ZHANG, Jun-Ling LU, Bing YANG
2021, 37(1): 140-150  doi: 10.11862/CJIC.2021.002
[摘要]  (69) [HTML全文] (69) [PDF 5116KB] (69)
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We systematically investigated Pd/FeOx for the reverse water gas shift (RWGS) reaction using a combination of ex situ and in situ characterizations, including transmission electron microscopy (TEM), Fourier-transform infrared (FTIR) spectroscopy, temperature-programmed desorption/reduction/oxidation (TPD/TPR/TPO), and X-ray photoelectron spectroscopy (XPS). A highly dispersed Pd/FeOx catalyst was synthesized using Pd(acac)2 as the precursor. The catalyst exhibited high activity, with CO2 conversion of ~29% and CO selectivity ogreater than 98% at 400℃, which are among the highest values in the literature. Moreover, Pd/SiO2 and Pd-Fe/SiO2 were further studied to determine the significant role of the Pd-FeOx interface in promoting the RWGS reaction. Semi-in situ XPS revealed the dynamic formation of Pdδ+-Fe2+ species at the Pd-FeOx interface; the species acted as highly active sites for CO2 dissociation. Our results also showed the formation of the Pdδ+-Fe2+ interface during the RWGS reaction remarkably enhanced the activity and selectivity of the Pd-FeOx catalyst for the reaction, benefiting CO2 adsorption, C=O dissociation, and CO desorption.
Aluminum Amine Compound Protected by β-Diketiminate Ligand: Preparation and Enhanced Performance as Catalyst for Ring-Opening Polymerization of ε-Caprolactone
Wen-Ling LI, Ben YAN, Chen-Guang SUN, Qiu-Miao SHEN, Wen-Qing LIU, Xiao-Li MA, Zhi YANG
2021, 37(1): 151-156  doi: 10.11862/CJIC.2021.007
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摘要:
An aluminum amine compound (L)AlH(NMe2) (L=HC(C(Me)NAr)2, Ar=2, 6-iPr2C6H3) (1) protected by steric β-diketiminate ligand L has been synthesized successfully. A two-step synthesis method was employed to prepare the aluminum amine (L)AlH(NMe2) compound. The aluminum amine compound (L)AlH(NMe2) was identified via NMR spectroscopy, elemental analysis, infrared diffuse reflectance spectroscopy and X-ray single crystal diffraction analysis. The aluminum amine compound containing both Al-NMe2 and Al-H substitutes showed excellent catalytic performance on the ring-opening polymerization of ε-caprolactone. The molecular weight and molecular weight distribution of the resultant polycaprolactone were determined by high performance gel penetration chromatography.
Easy Preparation of N-Doped Graphene-like Nanosheets as Excellent Metal-Free Cathodic Electrocatalysts of Zn-Air Battery
Xiao-Kun YANG, A-Ling CHEN, Qing-Feng YI
2021, 37(1): 157-170  doi: 10.11862/CJIC.2021.001
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Carbon-based materials have been paid much attention due to their own good electroactivity and resources availability. Herein, we reported a simple and versatile synthesis strategy for the preparation of nitrogen-doped and metal-free carbon catalysts with excellent oxygen reduction reaction (ORR) electroactivity. Using dicyandiamide (DCD) as nitrogen source and sucrose, β-cyclodextrin and chitosan as different carbon sources, N-doped graphene-like nanosheet samples CN-nanosh(suc), CN-nanosh(cyc) and CN-nanosh(ch) were prepared by an easy pyrolysis of their mixture. The samples exhibited outstanding ORR electroactivity in alkaline media with a comparable performance to the benchmark Pt/C. Alkaline Zn-air battery with the prepared sample CN-nanosh(suc) as the cathodic catalyst displayed the maximum power density of 201.33 mW·cm-2, and its discharge time can last for more than 50 h at a constant current density of 100 mA·cm-2, which is close to the optimum values of the similar Zn-air battery with the metal-free cathodic electrocatalysts reported so far.
Electrodeposition of NiS on CoNi2S4 for Flexible Solid-State Asymmetric Supercapacitors
Ye-Zeng HE, Hou-Qiang ZHAO, Peng LIU, Yan-Wei SUI, Fu-Xiang WEI, Ji-Qiu QI, Qing-Kun MENG, Yao-Jian REN, Dong-Dong ZHUANG
2021, 37(1): 171-179  doi: 10.11862/CJIC.2021.011
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摘要:
An effective approach of depositing NiS on CoNi2S4 was adopted to improve the performance of bimetallic cobalt/nickel-sulfide. The as-obtained CoNi2S4@NiS had an excellent specific capacitance of 1 433 F·g-1 at 1 A·g-1 and shows a superior rate performance of 69.6% at 10 A·g-1. A flexible solid-state asymmetric supercapacitor assembled with CoNi2S4@NiS and the reduced graphene oxide showed a high energy density of 36.6 Wh·kg-1 at a power density of 800 W·kg-1 and had a fantastic cycle performance of 78.7% retention after 10 000 cycles, indicating that the CoNi2S4@NiS nanocomposite is a promising electrode material for energy storage devices.
Preparation and in Vitro Experiment of Attapulgite-based Microgels with Magnetic/Temperature Dual Sensitivities
Tian-Le LI, Hui ZHONG, Xiao-Rong LI, Jing ZHOU, Yi-Xin LIU, Wei-Cheng HU, Zhi-Peng CHENG, Cheng YAO
2021, 37(1): 180-188  doi: 10.11862/CJIC.2021.017
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摘要:
The folic acid (FA)-grafted magnetic FA-Fe3O4/ATP-P(NIPAM-AAM) composite microgels (attapulgite=ATP, N-isopropyl acrylamide=NIPAM, acrylamide=AAM) were prepared via a method of emulsion copolymerization. The as-prepared microgels were characterized by X-ray diffraction (XRD), vibrating sample magnetometer (VSM), thermogravimetric analysis (TG), infrared spectroscopy (IR), UV-visible spectroscopy (UV), scanning electron microscope (SEM) and transmission electron microscope (TEM). The dynamic light scattering (DLS) results show that the low critical solution temperature (LCST) of microgel was about 38.5℃. The drug delivery ability of the as-prepared microgels was evaluated by using doxorubicin hydrochloride (DOX) as the model drug. Based on the drug loading and releasing results, the presence of ATP increased the amount of drug loading and releasing. Compared with free DOX, the in vitro cytotoxicity of DOX loaded FA-Fe3O4/ATP-P(NIPAM-AAM) was decreased and the biocompatibility was improved. Those results indicate that the microgels of FA-Fe3O4/ATP-P(NIPAM-AAM) can be used in potential as a slow-release drug system. The in vitro cellular uptake test revealed that the microgels of FA-Fe3O4/ATP-P(NIPAM-AAM) at the assigned site were significantly richer than that of other sites. This result indicates that the microgels of FA-Fe3O4/ATP-P(NIPAM-AAM) composite are targeting and expectable in the application of targeted drug releasing.
Errata
Correction to "Direct Observation of Magnetic Transitions in a Nickel(Ⅱ) Complex with Large Anisotropy"
N. Widener Chelsea, N. Bone Alexandria, Ozerov Mykhaylo, Richardson Rachael, Zheng-Guang LU, Thirunavukkuarasu Komalavalli, Smirnov Dmitry, Xue-Tai CHEN, Zi-Ling XUE
2021, 37(1): 189-189  doi: 10.11862/CJIC.2021.040
[摘要]  (76) [HTML全文] (76) [PDF 4212KB] (76)
摘要:

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