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应用核技术的海洋化学研究 【作者】陈绍勇 【导师】黄奕普

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~\ {bop0vt$`0应用核技术海洋化学研究
DFG|@s0Study of Marine Chemistry by Means Nucleus Technique

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yP%o(Ki4bw B]0作者】陈绍勇 【导师】黄奕普
2Bv S9\Hhm0【作者基本信息】厦门大学,海洋化学,2002年,博士水利论文ib'Qi8j_q4wy l

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fg0D~;?0【中文摘要】 本研究开展了多核素示踪剂的分离和海洋中金属元素除去机理以及海洋样品中铁的穆斯堡尔谱学研究。主要研究结果如下: 1.建立了从加速器产生的135Me V/u的12C、14N或16O离子束照射后的Au、Ag、Cu和Fe靶中分离多核素示踪剂的化学分离方法,使多核素示踪技术能够在严格一致的实验条件追踪各种环境、化学和生物系统的各种元素并比较它们的行为。所建立的利用阴离子交换树脂法从铁靶中分离出示踪剂的方法,全部化学流程只需约两小时,这对短半衰期核素的示踪研究起到关键性的作用。 2.氢氧化铁、深海沉积物、蒙脱石、近岸沉积物、高岭土对各种研究元素的吸附分配系数(Kads)大小有如下的顺序:氢氧化铁>深海沉积物>蒙脱石>近岸沉积物>高岭土。因此,可以认为铁和锰的氧化物和氢氧化物在对海洋中金属元素的除去机理上,比粘土矿物起着更重要的作用。获得了氢氧化铁、深海沉积物、蒙脱石、近岸沉积物、高岭土对金属元素的吸附分配系数(Kads)的对数和金属阳离子的电子结合能IZ关系图。金属元素的吸附分配系数与金属阳离子的电子结合能IZ之间存在Kads随IZ变化的关系表明,金属离子...更多的电子结合能是控制金属元素吸附的一个重要因子。金属元素的吸附分配系数的对数和平均海洋停留时间有良好的相关性,这表明,金属元素在颗粒物表面的吸附对它们从海洋中的除去过程起着重要的作用。从实验和理论上推导出金属元素的停留时间与吸附分配系数的相关关系。 3.采用选择性和非选择性的化学浸取的方法,研究了在化学 浸取前后深海沉积物、近岸沉积物和锰结核铁的穆斯堡尔谱。近 岸沉积物的穆斯堡尔谱包含了高自旋的顺磁性kZ\6叫.13mfors, AEq一2石smm/s)和顺磁性Fe’”(一0.35mln/s,AEq一0石4m血s);深海 沉积物的穆斯堡尔谱则包含了高自旋的顺磁性 F八顺磁性 F4“ 和磁性灭3“(6-0.4ffifors,H-510 KG)。虽然深海沉积物k 的总 含量高于近岸沉积物,但其Fey0e卜比值比近岸沉积物小,这主要 是山于深海沉积物中较高的自生的铁氧化物。此外,深海沉积物 中的铝硅酸盐的k\Fe3\值也小于近岸沉积物中铝硅酸盐的该 比值。这可能应归因于相对于近岸沉积物,深海沉积物中粘土矿 物含量和自生硅铝酸盐含量较高。锰结核的穆斯堡尔谱包含了高 自旋的顺 磁性 Fe’”(5-1.10mrn/s,凸Eq-2*Znun/s)和顺磁性 Fe3” O-0.35mm/s,AEq-0石smm/s),浸取后的锰结核铁的穆斯堡尔谱清 楚地显示含有Fey的特征穆斯堡尔谱,表明深海沉积物和锰结核中 reZ”组分是来源于大气降尘的陆源性物质。 4.应用 57Fe的穆斯堡尔谱学的方法研究了珠江口、南海东北 部和南沙群岛海域沉积物Fe的价态及相对组成。发现南海东北部 沉积物的穆斯堡尔谱包含了高自旋的顺磁性 Fey(6叫.12mm儿, 八和=2.64nun/s)和贝磁性Fe’”(6=0.36侧/s,A Eq二0.58mm/s), 而珠江日沉积物的穆斯堡尔谱除了这两组分外,还含有磁性组分 Fe几(6=0.37mm/S,H。。=506.OKG)。珠江日沉积物*”/Fe‘”的比 值和溶解态Fe含量与盐度的关系表明,在河口区混合过程中Fe 的行为是非保守的,溶解态的Fe是除去的。南沙群岛海域沉积物 的穆斯堡尔谱包含了高自旋的顺磁性k升(6叫.13。乃,和= 2.64*/S)、贝磁性h3”(6=0.36m/S,Eq=0.SSWh/S),黄铁矿 FeS。(6=0,32tTirn/s,冈=0。611.~------.-/s)和磁性组分 Fe。0.;(6 且互 。t ”0.37mm/s,H。=5 11.4KG)。所研究的三个海区,其穆斯堡尔谱组 成均不尽相同。 5.应用’丫e穆斯堡尔谱学研究了大亚湾浮游植物和合浦珠母 贝铁的化学状态和FC入”/”的比值。大亚湾浮游植物的穆斯堡尔谱 包含了高自旋的顺磁性k”(6叫.10Wb/S;凸成=2.63Th乃)和 顺磁性Fe’”(6=0.30m*,凸冈=0.64rum/s);合浦珠母贝的穆斯 堡尔谱包含了高自旋的顺磁性 Fey(6叫.13fnm乃,八冈=2.23fnm八) 和)i磁性 FC‘”(6=0.26Wb/S,A岛=0.67m/S)。合浦 珠母贝 Fe’”/Fe3”卜  还原

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【英文摘要】 Radiaochemical procedures by which prepare radioactive multitracer solutions, removal mechanisms of metal elements from seawater and MOssbauer spectroscopy in marine samples were studied in the present work. Main results are as follows:1.We established "multitracer" , a new versatile radiotracer technique, for simultaneous tracing of a number of elements in various chemical , environmental, and biological systems. Metal foil targets (typically Au, Ag, Ge, Cu and Fe) are irradiated with C, N, or 0 ions accelerated up to 135 Me V/nucleon by RIKEN Ring Cyclotron. Radiochemical procedures have been developed to remove the target material leaving the nuclides as Multitracer solutions containing various radionuclides of Be, Na, Mg, K, Ca, Sc V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Se, Br, Rb, Sr, Y, Zr, Nr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, In, Sn, Te, I, Ba, Ce, Pm, Eu, Gd, Tb, Tm, Yb, Lu, Hf, W, Re, Os, Ir, Pt, and Hg. Multiracers enable efficient tracing of a number of elements, and comparis...更多on of their behavior under strictly identical experimental conditions. Such features will be demonstrated by means of an example of application to a model experiment for the study of removal mechanism of various elements from the ocean.2 . Using radioactive multitracers produced by RIDEN Ring Cyclotron, the adsorption of metal elements on hydrated ferric oxide, marine sediments ( deep-sea and near-shore sediments ) and clay minerals (montmorillonite and kaolinite ) from artificial seawater was studied. The adsorption coefficients(Kads) of Mg, Sc, V, Mn, Fe, Co, Ni, Zn, Ca, As, Se Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, In, Sn, Eu, Gd, Tb, Tm, Yb, Lu, Hf, Re, and Hg were determined. The order of Kads for each element can be summarized as follows: hydrated ferric oxide > deep-sea sediment > montmorillinite > near-shore sediment > kaolinite. The observed relationships between log Lads and the logarithm of the mean oceanic residence time indicate that adsorption of metal elements on marine particulate materials plays an important role in their removal from seawater.3.The chemical states of iron in near-shore, deep-sea sediments and manganese nodule were investigated by means of n'Fe Mossbauer spectroscopy in combination with selective and non-selective chemical leachings. As far as a limited number of the sediments analyzed are concerned, Mossbauer spectra of near-shore sediments consist of high-spin paramagnetic ferrous(δ=1. 13mm/s ,ΔEq=2.65mm/s) and paramagnetic ferric(δ=0. 35mm/s, ΔEq=0. 64mm/s)components, while those of deep-sea sediments are composed of high-spin paramagnetic ferrous, paramagnetic ferric and magnetic ferric (δ 0. 4mm/s, H 510 KG) components. The Fe2V Fe3+ ratios of deep-sea sediments are much smaller than those in near-shore sediments, while the total concents of iron in the former are much higher than those in the latter. This is principally due to the high contents of authigenic ferric oxides in deep-sea sediments. Further, in the aluminosilicate fraction, the Fe2+/ Fe3* ratios of deep-sea sediments are also smaller than those of near-shore sediments. This is probably attributed to high contents of clay minerals and authigenic aluminosilicates in deep-sea sediments relative to near-shore ones. The magnetic components in deep-sea sediments are attributable to hematite, magnetite and/or maghematite. Mossbauer spectra of manganese nodule consist of high-spin paramagnetic ferrous(δ=1. lOmm/s , ΔEq=2.62mm/s) and paramagnetic ferric(δ=0. 35mm/s, ΔEq=0. 68mm/s). The former is much more pronounced in the spectrum of the sample after leaching. The ferrous component in the manganese nodule are shown to originate in terrigeous materials transported from lands through the atmosphere.4. The chemical states and relative concentrations of iron in the sediments from the Zhujiang River mouth, the northeastern South China Sea and Nansha sea area are studies by means of 57Fe Mossbauer spectroscopy. Mossbauer spectra of near-shore sediments consist of high-spin paramagnetic ferrous(δ=1.12mm/s, Δ  还原

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