在全球能源转型目标驱动下，协同开发多源生物质资源是实现循环经济的重要途径。互花米草（SA）作为入侵性海滨植物，其过度扩张威胁海岸生态系统；废弃猪骨（BP）因富含羟基磷灰石（HAP）和有机组分，不当处置易引发资源浪费与污染。本研究聚焦异质生物质（SA与BP）共热解技术，通过组分互补与矿物-碳协同效应制备多功能共热解生物炭，以突破单一原料热解产物孔隙率低、活性位点不足的瓶颈。植物基SA提供纤维素/木质素碳骨架，动物基BP贡献钙磷矿物相及含N/P/O有机组分，共热解过程中内源磷抑制碳损失并诱导矿物定向相变，耦合孔隙调控与活性位点暴露，从而强化生物炭对重金属/抗生素的吸附性能。研究进一步揭示矿物相变动力学与异质界面耦合机制，结合密度泛函理论（DFT）阐明污染物在矿物-碳界面的电子转移与配位机理，建立“宏观性能-微观机制”关联模型。本研究为多源生物质高值化利用提供新策略，推动环境修复材料的设计与开发，实现“以废治废”的循环经济目标。主要成果如下：

（1）以富含内源矿物HAP的猪骨为生物质原料，基于梯度热解策略（500、700、900 ℃）构筑系列猪骨炭材料（BP-5、BP-7、BP-9），系统探究温度梯度对内源HAP矿物相及有机蛋白组分形态的调控机制及其对Cu²⁺吸附性能的影响。结果表明，热解温度显著改变材料微观结构：通过低温诱导HAP与有机蛋白自掺杂形成“蓬松面包状”高活性载体，同时生成丰富的含N/P/O活性官能团（-PO₄^3-、-OH和-CONH₂）及活性B型-碳酸盐羟基磷灰石位点（CHAP(B)）；而高温则促使猪骨炭形貌结构向“纳米线状（BP-7）”和“纳米球状（BP-9）”转变，活性位点数量降低。DFT模拟计算方法证实，BP-5中-PO₄^3-、-OH和-CONH₂等官能团通过增强界面电子转移与配位作用显著提升对Cu²⁺的吸附能力，实验表明，BP-5在1 h内对Cu²⁺吸附效率达85%，并且有着最佳的吸附量，可达71.60 mg·g^-1。其吸附机制涵盖络合、离子交换、溶解-沉淀及静电吸引协同作用。FTIR与XRD分析进一步验证了猪骨内HAP矿相与有机组分的协同吸附路径。此外，BP-5在复杂环境（pH波动、无机离子竞争、有机质干扰）下仍保持高吸附稳定性。

（2）以富含内源Na的互花米草与富含内源HAP的猪骨为生物质原料，通过一步热解炭化法制备了共热解炭材料SA-BP-5，系统揭示内源HAP与Na的协同效应对Cu²⁺吸附的强化机制。结果表明，SA与BP共热解时，内源Na与HAP通过交联反应促进异质生物质协同转化，形成含N/P/O活性官能团、sp²石墨C及复合异质结构（C-HAP@Na和C-CHAP(B)@Na），显著提升材料吸附性能。SA-BP-5对Cu²⁺吸附容量达74.56 mg·g^-1，分别为单一SA-5和BP-5吸附容量的3.57和1.04倍。结合酸洗实验、FTIR/XRD表征及DFT模拟，证实复合异质结构通过增强界面电子转移与配位能力主导吸附过程，其机制涉及矿物溶解-沉淀、离子交换及表面络合协同作用。此外，SA-BP-5在受到环境pH变化、无机离子、有机质和不同实际水体的影响下，仍然能够保持较高的吸附活性，并表现出优异的再生吸附性能，证明共热解炭潜在的实用价值。

（3）进一步探究生物质原料配比与钾改性掺杂比对材料性能的调控机制。结果表明，在生物质配比为“SA:BP=1:2”和掺杂比为“生物质:KHCO₃=1:0.5”制备的钾改性共热解炭（SA-BP(1:2)-K0.5）具有最优孔隙结构与吸附性能，其对Cu²⁺和四环素（TC）的吸附容量分别达175.99与127.57 mg·g^-1。进一步研究发现，吸附Cu²⁺后的废弃炭（SA-BP(1:2)-K0.5-Cu50）对TC的二次吸附容量显著提升至347.59 mg·g⁻¹，较原始材料提高2.72倍。XPS分析表明，Cu²⁺以高活性含Cu位点形式固定于材料表面（Cu含量从0%增至3.24%），FTIR与XRD表征证实Cu²⁺通过络合与离子交换途径被稳定捕获，且材料优异的孔隙结构得以保留，为TC二次吸附提供活性界面。循环实验显示，SA-BP(1:2)-K0.5-Cu50经5次再生后对TC吸附效率仍保持64.9%，并展现出对复杂环境（pH波动、离子竞争）的强适应性。动态吸附实验进一步验证其在实际水体中对TC的高效去除潜力。本研究通过改性优化策略制备了优异钾改性共热解炭，实现了重金属和抗生素多污染物的协同去除与废弃吸附剂的高值化再利用，为多污染物靶向修复材料的开发提供了新思路。

Under the global drive for energy transition, the synergistic development of multi-source biomass resources represents a crucial pathway toward achieving a circular economy. Spartina alterniflora (SA), an invasive coastal plant, poses a significant threat to coastal ecosystems, while discarded pig bones (BP), rich in hydroxyapatite (HAP) and organic components, risk resource wastage and pollution if improperly managed. This study focuses on the co-pyrolysis of heterogeneous biomass (SA and BP) to produce multifunctional biochar, leveraging compositional complementarity and mineral-carbon synergistic effects to overcome the limitations of single-feedstock pyrolysis, such as low porosity and insufficient active sites. The plant-based SA provides a cellulose/lignin carbon framework, while the animal-based BP contributes calcium-phosphorus mineral phases and N/P/O-containing organic components. During the co-pyrolysis process, endogenous phosphorus inhibits carbon loss and induces directional mineral phase transformation, promoting pore regulation and exposure of active sites to enhance the adsorption performance of biochar for heavy metals and antibiotics. Furthermore, the study elucidates the mineral phase transformation dynamics and the heterogeneous interface coupling mechanism, supported by density functional theory (DFT) to reveal the electron transfer and coordination mechanisms of pollutants at the mineral-carbon interface. A macroscopic performance-microscopic mechanism correlation model is established. This research provides a novel strategy for the high-value utilization of multi-source biomass, promoting the design and development of environmental remediation materials and realizing the circular economy goal of “treating waste with waste”. The main findings are as follows:

(1) Using BP rich in endogenous HAP as a biomass feedstock, a gradient pyrolysis strategy (500, 700, and 900 °C) was applied to synthesize a series of biochar materials (BP-5, BP-7, and BP-9). The temperature-dependent regulation of the HAP mineral phase and organic protein component morphology, as well as their impact on Cu²⁺ adsorption performance, were systematically investigated. The results demonstrated that pyrolysis temperature significantly influenced the material's microstructure. At low temperatures, the self-doping of HAP with organic proteins formed a “fluffy bread-like” high-activity carrier, generating abundant N/P/O-containing functional groups (-PO₄^3-, -OH, and -CONH₂) and active B-type carbonated hydroxyapatite (CHAP(B)) sites. In contrast, high-temperature pyrolysis induced morphological transitions into “nanowire-like (BP-7)” and “nanosphere-like (BP-9)” structures, resulting in a reduction of active sites. Density functional theory (DFT) simulations confirmed that the -PO₄^3-, -OH, and -CONH₂ groups in BP-5 enhanced Cu²⁺ adsorption through interfacial electron transfer and coordination interactions. Experimental results indicated that BP-5 achieved an 85% Cu²⁺ adsorption efficiency within 1 h, with the best adsorption capacity, which can reach 71.60 mg·g^-1. The adsorption mechanism involved a synergistic combination of complexation, ion exchange, dissolution-precipitation, and electrostatic attraction. FTIR and XRD analyses further verified the collaborative adsorption pathways between the HAP mineral phase and organic components within the pig bone biochar. Moreover, BP-5 maintained excellent adsorption stability under complex environmental conditions, including pH fluctuations, competitive inorganic ions, and organic matter interference.

(2) The co-pyrolysis biochar (SA-BP-5) was prepared using sodium (Na)-rich SA and HAP-rich BP as biomass feedstocks through a one-step pyrolysis carbonization process. The synergistic effect of endogenous HAP and Na on the enhanced Cu²⁺ adsorption mechanism was systematically elucidated. The results showed that during the co-pyrolysis of SA and BP, endogenous Na and HAP facilitated the cross-linking reaction, promoting the synergistic conversion of heterogeneous biomass. This process generated N/P/O-containing functional groups, sp² graphitic carbon, and composite heterostructures (C-HAP@Na and C-CHAP(B)@Na), significantly improving the adsorption performance. The Cu²⁺ adsorption capacity of SA-BP-5 reached 74.56 mg·g^-1, which was 3.57 and 1.04 times higher than that of SA-5 and BP-5, respectively. Combined with acid washing experiments, FTIR/XRD characterization, and DFT simulations, the results confirmed that the composite heterostructure dominated the adsorption process by enhancing interfacial electron transfer and coordination capability. The adsorption mechanism involved mineral dissolution-precipitation, ion exchange, and surface complexation. Furthermore, SA-BP-5 maintained high adsorption activity and exhibited excellent regeneration performance under varying environmental conditions, including pH fluctuations, inorganic ions, organic matter, and different actual water bodies, demonstrating its potential practical value.

(3) Further exploration was conducted to investigate the regulation mechanism of biomass feedstock ratios and KHCO₃-modified doping ratios on material performance. The results demonstrated that the KHCO₃-modified co-pyrolysis biochar (SA-BP(1:2)-K0.5), prepared at an optimal biomass ratio of “SA:BP= 1:2” and a doping ratio of “biomass:KHCO₃ =1:0.5”, exhibited superior pore structure and adsorption performance. Its Cu²⁺ and tetracycline (TC) adsorption capacities reached 175.99 and 127.57 mg·g^-1, respectively. Notably, the adsorption capacity of the waste biochar after Cu²⁺ adsorption (SA-BP(1:2)-K0.5-Cu50) for TC significantly increased to 347.59 mg·g^-1, representing a 2.72-fold enhancement compared to the original material. XPS analysis confirmed the immobilization of Cu²⁺ as highly active Cu-containing sites on the biochar surface, with the Cu content increasing from 0% to 3.24%. FTIR and XRD characterizations further validated that Cu²⁺ was stably captured through complexation and ion exchange mechanisms, while the biochar’s excellent pore structure was retained, providing an active interface for TC secondary adsorption. The regeneration experiments demonstrated that SA-BP(1:2)-K0.5-Cu50 maintained 64.9% of its TC adsorption efficiency after five cycles and exhibited strong adaptability to complex environments with pH fluctuations and ion competition. Dynamic adsorption experiments further verified its high potential for TC removal in actual water bodies. This study proposed a modification optimization strategy to fabricate KHCO₃-modified co-pyrolysis biochar, achieving the synergistic removal of heavy metals and antibiotics, while realizing the high-value reuse of waste adsorbents. This offers a novel approach for the development of targeted remediation materials for multiple pollutants.

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