自從工業革命以來，人類對煤炭和石油等化石燃料的依賴導致大量二氧化碳排放到大氣中。大氣中二氧化碳含量的持續上升將對環境產生負面影響，包括全球暖化和海平面上升。為了因應這些困境，人們開始關切二氧化碳捕獲、利用和儲存（CCUS）技術的發展，這被認為是減少碳排放的一種有潛力的解決方案。二氧化碳轉化技術被視為二氧化碳減量技術中潛在有效的方法，其中環加成反應因其將二氧化碳轉化為具有經濟價值的環狀碳酸酯的潛力而受到廣泛關注。近年來，人們開發了多種用於環加成反應的觸媒，然而這些觸媒遇到了一些挑戰，包括高溫高壓要求、反應時間長、需要輔觸媒以及產物分離困難等，因此，迫切需要開發上述問題之環境友善觸媒。
在本研究中，使用簡單的熱解方法合成碘化物修飾生物炭觸媒(C400-XI, X = 0、2、4、6、8和10)。透過XRD、SEM、EA、XPS、FTIR、及比表面積分析儀等來鑑定觸媒的形態和物理化學特性。隨後，將這些製備的觸媒用於環加成反應以生產碳酸丙烯酯(PC)，再以GC-MS分析並計算轉化率和選擇性。其中，C400-8I表現出優異的催化性能，其PC產率達64.4%，這歸因於較好的碘化物含量和其表面豐富的羧酸基，有助於活化環氧化物的C-O鍵及促進開環反應。
為了優化熱解溫度並增強環加成性能，我們在保持恆定的碘化物含量同時改變熱解溫度製備CY-8I (Y = 400、500、600、700)觸媒。其中，C500-8I有最佳的性能，其PC產率達76.1%，這可能是由於有較高的CO2吸附能力和氮含量。為了增強觸媒上的含氧官能基，我們使用C500-8I作為基底，並使用過氧化氫或氫氧化鉀將其活化，分別產生HC500-8I和KC500-8I。研究結果顯示，KC500-8I表現出優異的環加成性能，其PC產率進一步提升至89.9%，這可能歸因於具有豐富的含氧官能基。
最後以實際海洋廢棄物(螃蟹殼)依照KC500-8I的合成方法製備觸媒(命名為KCS-8I)。在環氧丙烷(43 mmol)、觸媒(0.1800 g)、溫度90 ℃、CO2壓力(10 kg/cm2)、反應時間3 h的反應條件下，KCS-8I的碳酸丙烯酯產率達到約80.3%，證明了環加成過程的高效率。此外，KCS-8I在循環測試中表現出良好的可回收性和穩定性。

Since the Industrial Revolution, human reliance on fossil fuels like coal and oil has resulted in substantial emissions of carbon dioxide into the atmosphere. This persistent rise in atmospheric carbon dioxide levels has caused adverse environmental consequences, including global warming and sea level rise. In response to these challenges, the development of carbon dioxide capture, utilization, and storage (CCUS) technology has attracted attention as a promising solution to mitigate carbon emissions. Carbon dioxide conversion technology is regarded as a potentially effective approach among carbon dioxide reduction techniques. The cycloaddition reaction has garnered significant attention for its potential to convert carbon dioxide into very valuable cyclic carbonates. In the recent years, several catalysts have been developed for cycloaddition reactions. However, these catalysts encounter several challenges, including high temperature and pressure requirements, long reaction times, the need for auxiliary co-catalysts, and difficulties in product separation. To solve the aforementioned problems, there is an urgent demand for the development of eco-friendly catalysts without requirement for additional auxiliary co-catalysts.
In this research, iodide-modified biochars (named as C400-XI, X = 0, 2, 4, 6, 8, and 10) are synthesized by using a simple pyrolysis approach. The morphological and physicochemical characteristics of these catalysts are analyzed by XRD, SEM, EA, XPS, FTIR, N2 adsorption-desorption measurements, and CO2 adsorption analyses. Subsequently, these prepared catalysts are employed in the cycloaddition reaction to produce propylene carbonate. The resulting products are subjected to GC-MS analysis to determine conversion and selectivity. Among them, the C400-8I demonstrates the best catalytic performance, with the yield of propylene carbonate reaching ca. 64.4%. This can be attributed to its optimal iodide contents and the abundant presence of carboxylic acid groups on its surface, which effectively activate the C-O bond of the epoxide and facilitate ring opening.
To optimize the pyrolysis temperature and enhance cycloaddition performance, we further prepare the catalysts (denoted as CY-8I (Y = 400, 500, 600, 700)) by keeping a constant iodide content while varying the pyrolysis temperature. Among these catalysts, the C500-8I presents the most favorable performance, yielding ca. 76.1% of PC. This is likely due to its superior CO2 adsorption capacity and nitrogen contents. For the purpose of enhancing the oxygen-containing functional groups on catalysts, we further activate the C500-8I by using hydrogen peroxide or potassium hydroxide, resulting in HC500-8I and KC500-8I, respectively. The findings indicate that the KC500-8I exhibits the superior cycloaddition performance, with the yield of PC of ca. 89.9%. This is probably because of its abundant oxygen-containing functional groups.
Moreover, the iodide-modified biochars (denoted as KCS-8I) derived from marine wastes (i.e., crab shells) are synthesized via the same method of KC500-8I preparation. Under the reaction conditions involving propylene oxide (43 mmol), catalyst (0.1800 g), temperature of 90 °C, CO2 pressure (10 kg/cm2), and reaction time of 3 h, the propylene carbonate yield through KCS-8I achieves approximately 80.3%, demonstrating high efficiency in the cycloaddition process. Most importantly, the KCS-8I maintains favorable recyclability and stability during the cyclic tests.

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