碳酸盐结合硫酸盐记录海水硫酸盐的δ34S和δ18O: 来自南海南部礁相碳酸盐岩的启示*

doi:10.11978/2025241

热带海洋学报 ›› 2026, Vol. 45 ›› Issue (5): 178-198.doi: 10.11978/2025241CSTR: 32234.14.2025241

碳酸盐结合硫酸盐记录海水硫酸盐的δ³⁴S和δ¹⁸O: 来自南海南部礁相碳酸盐岩的启示^*

邸鹏飞¹^,²^,³(), 李牛¹^,²^,³, 宫尚桂⁴, Jörn Peckmann⁵, 王淑红¹^,³, 陈多福⁴, 颜文¹^,³()

¹ 中国科学院南海海洋研究所, 海洋与边缘海地质重点实验室, 广东广州 510301
² 三亚海洋生态环境工程研究院, 海南三亚 572025
³ 中国科学院大学, 北京 100049
⁴ 上海海洋大学, 海洋科学学院, 深渊科学与技术上海工程研究中心, 上海 201306
⁵ 汉堡大学, 地球系统研究与可持续性中心, 地质研究所, 德国汉堡 20146

收稿日期:2025-12-17 修回日期:2026-02-15 出版日期:2026-09-10 发布日期:2026-10-13
通讯作者: 颜文
作者简介:
邸鹏飞(1982―), 男, 河北省涞源县人, 副研究员, 博士, 主要从事海底冷泉原位观测与甲烷生物地球化学研究。email: pfd@scsio.ac.cn
*感谢匿名审稿专家提出的宝贵修改意见和建议。
基金资助:
国家重点研发计划项目(2021YFC3100600); 海南省重点研发计划项目(ZDYF2021SHFZ060); 中国科学院战略性先导科技专项(XDA13010102)

Carbonate-associated sulfate records seawater sulfate δ³⁴S and δ¹⁸O: insights from reef carbonate rocks in the southern South China Sea^*

DI Pengfei¹^,²^,³(), LI Niu¹^,²^,³, GONG Shanggui⁴, Jörn Peckmann⁵, WANG Shuhong¹^,³, CHEN Duofu⁴, YAN Wen¹^,³()

¹ Key Laboratory of Ocean and Marginal Sea Geology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China
² Sanya Institute of Ocean Eco-Environmental Engineering, Sanya 572025, China
³ University of Chinese Academy of Sciences, Beijing 100049, China
⁴ Shanghai Engineering Research Center for Hadal Science and Technology, College of Marine Sciences, Shanghai Ocean University, Shanghai 201306, China
⁵ Institute for Geology, Center for Earth System Research and Sustainability, Universität Hamburg, Hamburg 20146, Germany

Received:2025-12-17 Revised:2026-02-15 Online:2026-09-10 Published:2026-10-13
Contact: YAN Wen
Supported by:
National Key Research and Development Program of China(2021YFC3100600); Key Research and Development Plan of Hainan Province(ZDYF2021SHFZ060); Strategic Priority Research Program of the Chinese Academy of Sciences(XDA13010102)

摘要/Abstract

摘要：

碳酸盐结合硫酸盐(carbonate-associated sulfate, CAS)是重建古海水硫酸盐同位素演化与全球硫循环的重要代用指标, 但其在经历复杂成岩作用的礁灰岩中原始信号的保真度尚存争议。文章对南海南部美济礁南科1 (NK-1)井连续礁灰岩岩芯开展系统CAS含量、δ³⁴S_CAS和δ¹⁸O_CAS分析, 以评估成岩作用对CAS记录的影响。结果表明, 早期成岩作用显著降低CAS含量, 原生文石-高镁方解石相中含CAS高达5413mg·kg^-1, 而经淡水或海水成岩改造后CAS下降了60%~80%, 暴露面处因大气淋滤降至< 200mg·kg^-1。尽管如此, δ³⁴S_CAS在整个岩芯中高度稳定(20.1‰ ~ 24.7‰, 均值22.9‰), 与同期海洋重晶石δ³⁴S一致, 表明硫同位素信号可有效抵抗再结晶与白云石化等成岩扰动。相反, δ¹⁸O_CAS变化剧烈(7.1‰ ~ 15.0‰), 仅5Ma以来样品保留原始海水信号, 更老样品明显受成岩流体氧同位素交换影响。研究证实, 礁灰岩中的CAS能够可靠记录古海水δ³⁴S, 但δ¹⁸O_CAS用于古环境重建需谨慎。这一发现为高精度利用热带礁相沉积示踪硫循环历史提供了关键约束。

关键词: 与碳酸盐结合的硫酸盐(CAS), 硫氧同位素, 成岩作用, 礁灰岩, 南海

Abstract:

Carbonate-associated sulfate (CAS) is a key proxy for reconstructing the isotopic evolution of seawater sulfate and tracing global sulfur cycling through geologic time. However, the fidelity of primary CAS isotopic signals in reef limestones subjected to complex diagenetic alteration remains uncertain. We present a systematic analysis of CAS abundance, sulfur isotopes (δ³⁴S_CAS), and oxygen isotopes (δ¹⁸O_CAS) in a continuous reef limestone core (Well NK-1) from Meiji Atoll in the southern South China Sea to evaluate the impact of diagenesis on CAS records. Our results show that early diagenesis strongly reduces CAS concentrations: primary aragonite-high-Mg calcite phases contain up to 5413 mg·kg^-1 CAS, whereas freshwater and marine diagenetic alteration reduces CAS by 60% to 80%, with values dropping below 200 mg·kg^-1 at subaerial exposure surfaces due to meteoric leaching. Despite this substantial loss of sulfate, δ³⁴S_CAS remains remarkably stable throughout the core (20.1‰ to 24.7‰; mean 22.9‰) and aligns closely with coeval marine barite δ³⁴S, demonstrating that the original seawater sulfur isotope signature is robustly preserved even through intense recrystallization and dolomitization. In contrast, δ¹⁸O_CAS exhibits large variability (7.1‰ to 15.0‰), indicating high susceptibility to diagenetic overprint. Only samples younger than ~5 Ma retain primary seawater δ¹⁸O_CAS values; older samples have been significantly modified by oxygen isotope exchange with diagenetic fluids. This study confirms that CAS in reef limestones provides a reliable archive of past seawater δ³⁴S, but cautions against the uncritical use of δ¹⁸O_CAS for paleoenvironmental reconstruction without rigorous diagenetic screening. These findings offer critical constraints for high-resolution reconstructions of tropical marine sulfur cycling using reefal carbonate successions.

Key words: carbonate-associated sulfate, sulfur and oxygen isotopes, diagenesis, reef limestone, South China Sea

中图分类号:

P734.41

邸鹏飞, 李牛, 宫尚桂, Jörn Peckmann, 王淑红, 陈多福, 颜文. 碳酸盐结合硫酸盐记录海水硫酸盐的δ³⁴S和δ¹⁸O: 来自南海南部礁相碳酸盐岩的启示^*[J]. 热带海洋学报, 2026, 45(5): 178-198.

DI Pengfei, LI Niu, GONG Shanggui, Jörn Peckmann, WANG Shuhong, CHEN Duofu, YAN Wen. Carbonate-associated sulfate records seawater sulfate δ³⁴S and δ¹⁸O: insights from reef carbonate rocks in the southern South China Sea^*[J]. Journal of Tropical Oceanography, 2026, 45(5): 178-198.

图/表 9

图1

图2

图3

图4

图5

附表S1

礁相碳酸盐岩的残留水溶性硫酸盐和碳酸盐结合硫酸盐的含量、硫氧同位素比值与Mg/Ca、Mn/Sr值"

样品号	深度/m	WSS/(mg·kg^-1)	CAS/(mg·kg^-1)	δ³⁴S_WSS	δ¹⁸O_WSS	δ³⁴S_CAS	δ¹⁸O_CAS	Mg/Ca	Mn/Sr
0	0		5413			21.6	10.6	0.0479	0.0052
5	5.55	8	1527			22.8	11.5	0.0505	0.0060
52	10.25	218	4511	19.8	11.8	22.9	10.8	0.0448	0.0050
152	20.85	2	301			20.5	8.6	0.0075	0.0139
221	28.32		354					0.0090	0.5256
262	32.44		399			20.8	9.0	0.0049	0.0472
303	38.83		249					0.0061	0.0353
319	40.43		358					0.0058	0.0372
342	43.75	3						0.0054	0.0318
351	43.67		372			21.7	9.9	0.0044	0.0318
450	53.83	54	210	20.1	9.8	22.4	10.4	0.0044	0.0303
517	60.57		456					0.0047	0.0011
531	62.39	4	411			21.7	9.2	0.0050	0.0123
571	67.53		227					0.0054	0.0268
602	71.05	1	211			20.1	9.4	0.0066	0.0244
692	80.11	2	379			20.8	9.3	0.0077	0.0483
750	85.95		92					0.0104	0.0544
759	86.85		405					0.0105	0.0793
795	92.47	33	226			22.1	10.7	0.0106	0.0422
813	92.27		133					0.0093	0.0244
862	97.33		493					0.0097	0.0167
895	100.63	1	207			23.4		0.0113	0.019
978	108.99	20	942			23.4	12.4	0.0241	0.0290
1074	118.65		475			22.8	11.0	0.0143	0.0545
1080	119.27	26	325					0.1671	0.1767
1103	121.59		1055					0.4576	0.1922
1189	130.23	1	1127			23.0	12.2	0.2282	0.1438
1264	138.19		1272					0.4499	0.1082
1278	139.81		1310			22.7	11.4	0.4458	0.1106
1301	142.11	1	1154					0.4600	0.1128
1377	149.77		902			23.0	12.8	0.4844	0.1181
1388	150.87		849					0.5142	0.1738
1443	156.91	3	1117			24.1	10.6	0.4249	0.1123
1513	164.33		614					0.5611	0.1717
1533	166.33		598					0.5054	0.0938
1545	166.93	2	1137			23.1	12.0	0.4714	0.0971
1556	170.03		735					0.5259	0.0971
1593	171.73		726					0.5197	0.1736
1628	175.33	2	420					0.5507	0.2234
1687	181.23		466			23.5	11.8	0.5252	0.1501
1728	185.43	1	953					0.4385	0.1216
1739	186.53		884					0.0066	1.1945
1759	188.53		1092					0.5239	0.346
1769	189.53		925			22.1	12.2	0.5364	0.4544
1790	191.63		608					0.5445	0.2218
1812	193.83		390					0.5788	0.4373
1834	196.13	264						0.5798	0.5538
1857	201.33		798			20.4	10.5	0.5847	0.5791
1881	203.93	151		16.1	8.4			0.5846	0.3278
1909	206.83		503					0.5816	0.29
1933	209.23		604					0.5859	0.317
1952	211.13	279	528	12.6	8.2	23.4	11.5	0.5604	0.3441
1959	211.83		801			23.5	11.8	0.5604	0.3441
1982	214.23		1294					0.5226	0.3739
1993	215.53		1161					0.5226	0.3136
2030	220.33		617					0.5853	0.2537
2046	222.13	232	529					0.5822	0.2469
2063	223.83		953			20.8	10.5	0.5706	0.2401
2095	227.03		693					0.5343	0.2580
2104	227.93		1672					0.5110	0.2437
2123	229.93		1363					0.5110	0.2294
2133	230.93	8	925					0.5110	0.2551
2161	234.33		770					0.5516	0.2809
2167	235.03		1655					0.4761	1.0035
2176	236.13					22.1	10.8	0.4750	0.8440
2200	238.53		1368					0.4725	0.4572
2205	239.03		1322					0.5125	0.4024
2217	240.23		886					0.5125	0.3475
2227	241.23	2	790					0.5242	0.3129
2259	244.53		888			23.8	11.9	0.5481	0.2784
2323	251.73	123	247					0.5903	0.4173
2337	255.53		747					0.5748	0.9726
2383	260.63	41	477					0.5895	1.1956
2406	262.93		613					0.5848	0.4771
2414	263.73		717					0.5848	0.4683
2423	264.63		572					0.5950	0.4595
2443	266.63		319					0.5935	0.5088
2452	267.48	81	513	18.2	9.7	22.2	11.2	0.5943	0.4842
2478	270.13		578					0.5979	0.5086
2548	279.68	136	1026	20.3	10.1	21.1	9.0	0.5921	0.4743
2599	286.03		1052					0.5619	0.4296
2612	287.33		748					0.5619	0.4173
2641	290.13	4	908					0.4943	0.3622
2651	291.13		873			22.8	12.5	0.5164	0.3836
2657	291.73		900					0.5385	0.4228
2670	293.13		595					0.5385	0.4955
2711	297.23	113	392	19.1		23.4	12.0	0.5627	0.5460
2752	301.33		619					0.5584	0.4359
2762	302.33		617					0.5104	0.3722
2794	305.53		206					0.4797	0.2535
2804	306.53	3	813					0.4797	0.226
2814	307.53		1109			23.3	13.1	0.4797	0.1984
2823	308.43		1278					0.4797	0.1733
2897	315.93		910					0.4960	0.1460
2919	318.13	1	1351			23.0	12.6	0.4940	0.1243
2937	319.93		1024					0.4920	0.1287
2968	323.23		1099					0.5000	0.4547
2987	325.23		798					0.5401	0.116
3019	329.43		990			23.2	13.5	0.4749	0.0754
3032	330.73	4						0.5271	0.1372
3063	333.83		731					0.4889	0.0905
3072	334.73		292					0.5518	0.0946
3112	338.83		345			22.1	11.1	0.4736	0.0584
3145	342.13	1	1025					0.4672	0.1048
3157	343.33		1043					0.4766	0.0619
3222	351.53		987			22.6	11.5	0.4792	0.0580
3224	351.73					24.1	11.3	0.4792	0.0580
3231	352.43	1	744					0.4792	0.0569
3244	353.93		964					0.4911	0.0558
3292	358.73		497					0.5343	0.0941
3312	360.73	3	646					0.4855	0.0788
3337	363.33		1242			23.1	12.1	0.4656	0.0998
3398	370.23	21						0.4719	0.1091
3433	373.73	12	1129			23.7		0.4812	0.1299
3506	381.03	6	1341					0.4594	0.0787
3543	385.23	1	1205			22.7	12.7	0.4576	0.0476
3672	399.73	20	1393			23.5	11.3	0.4932	0.1555
3693	401.83	1	1116			23.6	11.1	0.4875	0.2074
3733	405.83		957					0.4838	0.2301
3752	407.73		616					0.4833	0.1345
3788	411.73	37	1202	14.9	9.4	22.3	12.6	0.4629	0.0735
3819	414.83		1256			22.9	12.2	0.4773	0.0924
3882	421.13	12						0.4581	0.0540
3923	425.23		1147			23.4	12.7	0.4662	0.0553
3973	429.83	8	979					0.4685	0.0611
4028	435.73	1	524			24.2	12.8	0.4791	0.0665
4134	449.83	173	975	23.5	13.8			0.4503	0.0471
4149	452.62		966			23.9	11.9	0.4650	0.0420
4168	454.63		1173			23.1	13.1	0.4796	0.0369
4179	455.63		1170					0.4260	0.0322
4194	457.13	87	1015					0.4260	0.0276
4242	465.03		1129			23.5	12.4	0.4604	0.0653
4271	467.93	3	647					0.1986	0.0425
4351	479.63	1	917			23.3	12.8	0.2450	0.0444
4463	497.53	4	560			23.7	11.2	0.4132	0.0590
4536	507.13		681					0.4562	0.0126
4613	515.63		857					0.4590	0.1355
4636	518.13		1007					0.4663	0.1695
4669	523.03		951			23.4	13.5	0.4715	0.0808
4707	526.83	101	978					0.4821	0.1937
4772	533.43		1242			23.7	10.7	0.4719	0.2643
4798	536.03	2	1008					0.4726	0.2177
4850	541.23	4	471					0.0088	0.6386
4895	545.73	24				21.5	10.1	0.0106	0.3076
4963	552.53	1	443			23.0	15.0	0.0188	0.0474
5056	562.73					22.9	13.3	0.0143	0.2500
5140	571.73		433			23.4	11.9	0.0263	0.0541
5170	574.73	34						0.0226	0.3442
5245	582.23	1	1119			24.0	13.1	0.0225	0.0327
5341	591.83	74	1346	21.5	13.0	23.5	13.2	0.0265	0.0239
5419	599.73	1	991			23.1	12.7	0.0229	0.3355
5587	616.73		839			23.5	12.4	0.0089	0.4750
5608	618.83	4	326			22.6	9.2	0.0075	0.1327
5619	619.93		582					0.0054	0.0023
5654	623.43					23.7	12.5	0.0141	0.1497
5724	630.43	20	1137			23.2	11.7	0.0166	0.0583
5750	633.13		2001			24.7	7.1	0.0200	0.1447
5759	634.03		967					0.0188	0.4508
5786	636.83		728					0.0218	0.1256
5866	645.03	3	1505			23.0	12.0	0.0239	0.1562
5882	646.63		1530					0.0222	0.3832
5935	651.93	17	1373					0.0190	0.2412
5994	657.83	12	2725			22.9	12.3	0.0206	0.1704
6096	668.05		1133			23.3	11.6	0.0173	0.0662
6104	668.85	14	1068			23.4	10.3	0.0142	0.6301
6141	672.55		968					0.0188	0.2257
6152	673.65	10	142			23.6	12.0	0.0200	0.3113
6270	685.45	82	1510			24.3	10.9	0.0205	0.5868
6272	685.65		1156					0.0205	0.5868
6331	691.55		1487					0.0173	0.4856
6357	694.15	22	1245			23.6	11.6	0.0203	0.0739
6405	698.95		1167					0.0207	0.6439
6452	703.65	2	1234			23.4	12.4	0.0194	0.1085
6553	713.75	20						0.0198	0.3295
6573	715.75		1217			23.9	10.1	0.0183	0.4893
6654	723.85	1	1065			23.4	12.2	0.0189	0.9490
6674	725.85		1215					0.0198	0.1756
6770	735.45		1598					0.0209	0.168
6779	736.35					23.1	12.8	0.0209	0.1275
6829	741.35		961					0.0172	0.0970
6837	742.15		762			22.2	11.4	0.0172	0.0761
6862	744.65	5	1485					0.0172	0.0604
6890	745.45		1260					0.0193	0.0658
6914	749.85	82		21.3	12.9			0.0224	0.3192
6923	750.75		438			24.0	12.0	0.0224	0.2384
6941	752.55		1257					0.0206	0.1575
6951	753.55	61	912					0.0164	0.1359
6972	757.65		1085					0.0172	0.0672
7005	758.95	74						0.0182	0.0451
7051	763.55	45	1507			23.8	11.9	0.0205	0.0720
7107	769.15		1163					0.0163	0.0863
7118	770.25		1275					0.0198	0.0973
7133	771.75		1126					0.0172	0.0799
7145	772.95	1	855					0.0166	0.0835
7208	779.25		1164					0.0188	0.0596
7249	783.35	1	1233			23.3	13.0	0.0204	0.0602
7261	784.55		589					0.0191	0.0887
7373	798.75	1	922			23.8	12.9	0.0172	0.1811
7410	799.45		1610					0.0172	0.3006
7432	801.65	45	1143			23.3	11.8	0.0172	0.0842
7464	804.85		1080					0.0189	0.0947
7496	808.05	69	1184			23.4	13.0	0.0219	0.5754
7667	825.15	4	874			23.1	11.2	0.0176	0.3766
7703	828.75		1107					0.0180	0.1302
7745	832.95					23.3	11.8	0.0158	0.0824
7778	836.25	1	795			22.9	12.3	0.0199	0.0771
7792	837.65		950					0.0161	0.8336
7850	843.45		1209					0.0266	0.0749
7865	844.95	65						0.0184	0.0749
7873	845.75		777			23.0	12.5	0.0184	0.0749
7927	851.15	1	977					0.0159	0.1382
7992	857.65	25				23.7	11.0	0.0177	0.5625
8011	859.55	4						0.0184	0.2217
8045	862.95		1216			23.3	11.5	0.0224	0.5272
8103	868.75		2249					0.0224	0.1374
8128	871.25	25	2206			22.1	11.6	0.0173	0.0199
8217	880.15	62	1049			23.3	12.7	0.0234	0.5316
8249	883.35		695					0.0219	0.0778
8264	884.85		999					0.0233	0.5928
8314	889.85	124	1327	20.1	10.6	22.3	11.3	0.0150	0.0895
8386	897.05		683					0.0153	0.1135
8418	900.45	328	1403	19.6	10.2	21.8	11.0	0.0163	0.1104
8440	902.65		1368					0.0160	0.0635
8489	908.75	223						0.0157	0.0618
8526	912.45		1567			22.1	13.0	0.0155	0.0515
8545	914.35		1322					0.0152	0.0366
8615	922.05	53	1079					0.0151	0.0543
8616	922.15		486					0.0151	0.0481
8622	922.75		803					0.0158	0.0418
8643	924.85		1379			22.7	12.3	0.0158	0.0704
8702	930.75	261	1319					0.0135	0.1475
8716	932.15		1032					0.0156	0.1040
8730	933.55		1100			22.2	11.1	0.0156	0.0605
8758	936.95		1292					0.0156	0.0691
8782	939.35		851					0.0144	0.0687
8803	941.45		1110					0.0155	0.0355
8835	944.65		938					0.0153	0.0356
8836	944.75		1288					0.0153	0.0330
8843	945.45	47	1097	21.5	11.0	23.5	10.8	0.0153	0.0329
8960	957.15		1276			23.4	12.0	0.0147	0.0531
8996	960.75	522	899	19.2	10.2			0.0145	0.0330
9052	966.35		1159			22.6	11.1	0.0159	0.0576
9072	968.35	251	1389	19.2	10.7	21.3	11.0	0.0140	0.0553
9127	973.85		1159			21.9	11.4	0.0137	0.0786
9161	977.25	366	1389			22.7	12.1	0.0152	0.1258

附表S1

图6

图7

图8

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碳酸盐结合硫酸盐记录海水硫酸盐的δ³⁴S和δ¹⁸O: 来自南海南部礁相碳酸盐岩的启示^*

Carbonate-associated sulfate records seawater sulfate δ³⁴S and δ¹⁸O: insights from reef carbonate rocks in the southern South China Sea^*

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