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Instruments / Technical Area	Publication Details	Published
I08-Scanning X-ray Microscopy beamline (SXM)	Long-term organic carbon preservation enhanced by iron and manganese Oliver W. Moore , Lisa Curti , Clare Woulds , James A. Bradley , Peyman Babakhani , Benjamin J. W. Mills , William B. Homoky , Ke-Qing Xiao , Andrew W. Bray , Ben J. Fisher , Majid Kazemian , Burkhard Kaulich , Andrew W. Dale , Caroline L. Peacock Nature 178 DOI: 10.1038/s41586-023-06325-9 Diamond Proposal Number(s): [18560, 21323] Open Access Show Abstract ▼ Abstract: The balance between degradation and preservation of sedimentary organic carbon (OC) is important for global carbon and oxygen cycles1. The relative importance of different mechanisms and environmental conditions contributing to marine sedimentary OC preservation, however, remains unclear2,3,4,5,6,7,8. Simple organic molecules can be geopolymerized into recalcitrant forms by means of the Maillard reaction5, although reaction kinetics at marine sedimentary temperatures are thought to be slow9,10. More recent work in terrestrial systems suggests that the reaction can be catalysed by manganese minerals11,12,13, but the potential for the promotion of geopolymerized OC formation at marine sedimentary temperatures is uncertain. Here we present incubation experiments and find that iron and manganese ions and minerals abiotically catalyse the Maillard reaction by up to two orders of magnitude at temperatures relevant to continental margins where most preservation occurs4. Furthermore, the chemical signature of the reaction products closely resembles dissolved and total OC found in continental margin sediments globally. With the aid of a pore-water model14, we estimate that iron- and manganese-catalysed transformation of simple organic molecules into complex macromolecules might generate on the order of approximately 4.1 Tg C yr−1 for preservation in marine sediments. In the context of perhaps only about 63 Tg C yr−1 variation in sedimentary organic preservation over the past 300 million years6, we propose that variable iron and manganese inputs to the ocean could exert a substantial but hitherto unexplored impact on global OC preservation over geological time.	Aug 2023
I08-Scanning X-ray Microscopy beamline (SXM)	Diffuse hydrothermal venting: A hidden source of iron to the oceans Alastair J. M. Lough , Douglas P. Connelly , William B. Homoky , Jeffrey A. Hawkes , Valerie Chavagnac , Alain Castillo , Majid Kazemian , Ko-Ichi Nakamura , Tohru Araki , Burkhard Kaulich , Rachel A. Mills Frontiers In Marine Science 6 DOI: 10.3389/fmars.2019.00329 Diamond Proposal Number(s): [12738] Open Access Show Abstract ▼ Abstract: Iron (Fe) limits primary productivity and nitrogen fixation in large regions of the world’s oceans. Hydrothermal supply of Fe to the global deep ocean is extensive; however, most of the previous work has focused on examining high temperature, acidic, focused flow on ridge axes that create “black smoker” plumes. The contribution of other types of venting to the global ocean Fe cycle has received little attention. To thoroughly understand hydrothermal Fe sources to the ocean, different types of vent site must be compared. To examine the role of more diffuse, higher pH sources of venting, a hydrothermal plume above the Von Damm vent field (VDVF) was sampled for Total dissolvable Fe (unfiltered, TDFe), dissolved Fe (<0.2 μm, dFe) and soluble Fe (<0.02 μm, sFe). Plume particles sampled in situ were characterized using scanning electron microscopy and soft X-ray spectromicroscopy. The VDVF vents emit visibly clear fluids with particulate Fe (TDFe-dFe, >0.2 μm) concentrations up to 196 nmol kg–1 comparable to concentrations measured in black smoker plumes on the Mid-Atlantic Ridge. Colloidal Fe (cFe) and sFe increased as a fraction of TDFe with decreasing TDFe concentration. This increase in the percentage of sFe and cFe within the plume cannot be explained by settling of particulates or mixing with background seawater. The creation of new cFe and sFe within the plume from the breakdown of pFe is required to close the Fe budget. We suggest that the proportional increase in cFe and sFe reflects the entrainment, breakdown and recycling of Fe bearing organic particulates near the vents. Fe plume profiles from the VDVF differ significantly from previous studies of “black smoker” vents where formation of new pFe in the plume decreases the amount of cFe. Formation and removal of Fe-rich colloids and particles will control the amount and physico-chemical composition of dFe supplied to the deep ocean from hydrothermal systems. This study highlights the differences in the stabilization of hydrothermal Fe from an off-axis diffuse source compared to black smokers. Off-axis diffuse venting represent a potentially significant and previously overlooked Fe source to the ocean due to the difficulties in detecting and locating such sites.	Jul 2019
I08-Scanning X-ray Microscopy beamline (SXM)	Soluble iron conservation and colloidal iron dynamics in a hydrothermal plume A. J. M. Lough , W. B. Homoky , D. P. Connelly , S. A. Comer-Warner , K. Nakamura , M. K. Abyaneh , B. Kaulich , R. A. Mills Chemical Geology DOI: 10.1016/j.chemgeo.2019.01.001 Diamond Proposal Number(s): [12738] Open Access Show Abstract ▼ Abstract: Iron (Fe) limits or co-limits primary productivity and nitrogen fixation in large regions of the world's oceans, and the supply of Fe from hydrothermal vents to the deep ocean is now known to be extensive. However, the mechanisms that control the amount of hydrothermal Fe that is stabilized in the deep ocean, and thus dictate the impact of hydrothermal Fe sources on surface ocean biogeochemistry, are unclear. To learn more, we have examined the dispersion of total dissolvable Fe (TDFe), dissolved Fe (dFe) and soluble Fe (sFe) in the buoyant and non-buoyant hydrothermal plume above the Beebe vent field, Caribbean Sea. We have also characterized plume particles using electron microscopy and synchrotron based spectromicroscopy. We show that the majority of dFe in the Beebe hydrothermal plume was present as colloidal Fe (dFe − sFe = cFe). During ascent of the buoyant plume, a significant fraction of particulate Fe (pFe = TDFe − dFe) was lost to settling and exchange with colloids. Conversely, the opposite was observed in the non-buoyant plume, where pFe concentrations increased during non-buoyant plume dilution, cFe concentrations decreased apparently due to colloid aggregation. Elemental mapping of carbon, oxygen and iron in plume particles reveals their close association and indicates that exchanges of Fe between colloids and particles must include transformations of organic carbon and Fe oxyhydroxide minerals. Notably, sFe is largely conserved during plume dilution, and this is likely to be due to stabilization by organic ligands, in contrast to the more dynamic exchanges between pFe and cFe. This study highlights that the size of the sFe stabilizing ligand pool, and the rate of iron-rich colloid aggregation will control the amount and physico-chemical composition of dFe supplied to the ocean interior from hydrothermal systems. Both the ligand pool, and the rate of cFe aggregation in hydrothermal plumes remain uncertain and determining these are important intermediate goals to more accurately assess the impact of hydrothermalism on the ocean's carbon cycle.	Jan 2019

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