Abstract

Enhanced weathering of (ultra)basic silicate rocks such as olivine-rich dunite has been proposed as a large-scale climate engineering approach. When implemented in coastal environments, olivine weathering is expected to increase seawater alkalinity, thus resulting in additional CO2 uptake from the atmosphere. However, the mechanisms of marine olivine weathering and its effect on seawater–carbonate chemistry remain poorly understood. Here, we present results from batch reaction experiments, in which forsteritic olivine was subjected to rotational agitation in different seawater media for periods of days to months. Olivine dissolution caused a significant increase in alkalinity of the seawater with a consequent DIC increase due to CO2 invasion, thus confirming viability of the basic concept of enhanced silicate weathering. However, our experiments also identified several important challenges with respect to the detailed quantification of the CO2 sequestration efficiency under field conditions, which include nonstoichiometric dissolution, potential pore water saturation in the seabed, and the potential occurrence of secondary reactions. Before enhanced weathering of olivine in coastal environments can be considered an option for realizing negative CO2 emissions for climate mitigation purposes, these aspects need further experimental assessment.

Highlights

  • Climate engineering approaches that aim to deliberately and actively remove greenhouse gases from the atmosphere are categorized as carbon dioxide removal (CDR) or negative emission technologies (NETs).[1]

  • We address a number of questions related to the application of enhanced silicate weathering in natural coastal environments: (1) What is the rate of olivine dissolution in natural seawater and how does this differ from artificial seawater? (2) Does olivine dissolve stoichiometrically in natural seawater? (3) What dissolution products can be used to efficiently monitor the dissolution rate of olivine in coastal sediments, i.e., quantify the efficiency of enhanced silicate weathering? (4) To what extent does secondary mineral formation diminish the CO2 sequestration efficiency of olivine dissolution in seawater?

  • While ΔTA remained constant with time, ΔDIC decreased with 22 μmol kg−1 during the first 15 days, likely caused by CO2 outgassing, as the initial solution in A1 may not have been in equilibrium with the atmosphere

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Summary

Introduction

Climate engineering approaches that aim to deliberately and actively remove greenhouse gases from the atmosphere are categorized as carbon dioxide removal (CDR) or negative emission technologies (NETs).[1]. Enhanced silicate weathering (ESW) is a NET approach in which the natural process of (silicate) rock weathering is artificially stimulated.[5,6] The technique has been recognized as a potentially promising strategy for CO2 removal from the atmosphere while at the same time counteracting ocean acidification.[1,6−9] The implementation of ESW requires suitable source rock to be mined, ground to small grain sizes, and subsequently spread over suitable areas.[5] The mineral grains dissolve (i.e., chemical weathering), through which CO2 is eventually captured from the atmosphere.[6,10] Olivine (Mg2−xFexSiO4) is an abundant and fast-weathering ultramafic silicate mineral and has been advanced as a prime candidate mineral for ESW application.[5,11] The dissolution of olivine in an aqueous environment consumes protons or increases alkalinity,[6,12,13] and so increases CO2 uptake by the aqueous medium (Supporting Information section 1)

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