Methods and systems for reducing greenhouse gas emissions from sediments containing organic materials via treatment with lime are disclosed herein. In some embodiments, the method comprises (i) providing sediments comprising a first pH less than 10.0, fermentable organic materials, and microbes configured to produce carbon dioxide and/or methane via degradation of the organic material; (ii) adding a coagulant comprising lime to the sediment to produce a mixture comprising a second pH of at least 11.0 and excess soluble calcium ions; and (iii) after adding the coagulant, forming a buffer comprising soluble sodium and calcium bicarbonates within the mixture by enabling the excess soluble sodium and calcium ions to react with carbon dioxide. Forming the buffer can comprise decreasing the pH of the mixture from the second pH to a third pH of 8.0 or greater.