Shamim Haider

Industrial scale production of carbon membrane is very challenging due to expensive precursor materials and a multi-step process with several variables to deal with. The optimization of these variables is essential to gain a competent carbon membrane (CM) with high performance and good mechanical properties. In this paper, a pilot scale system is reported that was developed to produce CM from regenerated cellulose precursor with the annual production capacity 700 m² of CM. The process was optimized to achieve maximum yield (>95%) of high quality precursor fibers and carbonized fibers. A dope solution of cellulose acetate (CA)/Polyvinylpyrrolidone (PVP)/N-methyl-2-pyrrolidone (NMP) and bore fluid of NMP/H₂O were used in 460 spinning-sessions of the fibers using a well-known dry/wet spinning process. Optimized deacetylation of spun-CA hollow fibers (CAHF) was achieved by using 90 vol% 0.075 M NaOH aqueous solution diluted with 10 vol% isopropanol for 2.5 h at ambient temperature. Cellulose hollow fibers (CHF) dried at room temperature and under RH (80% → ambient) overnight gave maximum yield for both dried CHF, as well as carbon fibers. The gas permeation properties of carbon fibers were also high (CO₂ permeability: 50–450 Barrer (1 Barrer = 2.736 × 10⁻⁹ m³ (STP) m/m² bar h), and CO₂/CH₄ selectivity acceptable (50–500).

The simultaneous carbonization of thousands of fibers in a horizontal furnace may result in fused fibers if carbonization residuals (tars) are not removed fast enough. The optimized purge gas flow rate and a small degree angle in the furnace position may enhance the yield of high quality carbon fibers up to 97% by removing by-products. The production process for several thousand carbon fibers in a single batch is reported. The aim was developing a pilot-scale system to produce carbon membranes. Cellulose-acetate fibers were transformed into regenerated cellulose through a de-acetylation process and the fibers were carbonized in a horizontally oriented three-zone furnace. Quartz tubes and perforated stainless steel grids were used to carbonize up to 4000 (160 cm long) fibers in a single batch. The number of fused fibers could be significantly reduced by replacing the quartz tubes with perforated grids. It was further found that improved purge gas flow distribution in the furnace positioned at a 4-degree to 6-degree angle permitted residuals to flow downward into the tar collection chamber. In total, 390 spun-batches of fibers were carbonized. Each grid contained 2000–4000 individual fibers and these fibers comprised four to six spun-batches of vertically dried fibers. Gas permeation properties were investigated for the carbon fibers.