Spontaneous energy-harvesting from the environment without external stimuli is a challenging task for clean and renewable power. However, existing carbon-based energy generators require the sequential gradient structure and can only produce a low and desultory power relying on the atmospheric moisture. Here we develop a direct dry-compression molding strategy to rapidly manufacture the heterostructured F/O-bonded graphene monolith (H-OGF) with two integrated parts of fluorinated oxidized graphene (FOG) and oxidized graphene (OG) for the first time. Fabricated H-OGF device spontaneously generates a voltage of ~1.25 V (the largest voltage reported for spontaneous carbon-based energy-harvesting devices) and it also achieves a continuous power output for external resistance over 40,000 s with good stability and recyclability. The initial energy input is originated from the transformation of moisture from the gaseous state in atmosphere to the agminated state in H-OGF. This promotes the H⁺ dissociation and the spontaneous formation of self-maintained and huge H⁺ concentration difference between FOG and OG layers, which works as the driving force for the continuous power production. Moreover, the introduced fluorine with the maximal electronegativity (3.98) accelerates the carboxyl’s ionization and further magnifies H⁺ concentration difference. Connecting several H-OGF devices proportionally amplifies voltage up to 10 V for powering electronics and obtains a wearable power supply. Our findings make H-OGF devices promising candidates for low-budget and self-sustaining energy systems as rigorous requirement of location or environmental conditions is loosened.

在没有外部刺激的情况下从环境中自发收集能量对于清洁和可再生能源来说是一项具有挑战性的任务。然而，现有的碳基能源发电机需要顺序梯度结构，只能依靠大气水分产生低强度和断断续续的电力。在这里，我们开发了一种直接干压成型策略，以首次快速制造具有氟化氧化石墨烯 (FOG) 和氧化石墨烯 (OG) 两个集成部分的异质结构 F/O 键合石墨烯整体 (H-OGF)。制造的 H-OGF 装置自发产生约 1.25 V 的电压（自发碳基能量收集装置报道的最大电压），并且它还实现了超过 40,000 秒的外部电阻连续功率输出，具有良好的稳定性和可回收性。初始能量输入源于水分从大气中的气态转变为 H-OGF 中的凝聚态。这促进了 H⁺解离以及FOG 和 OG 层之间自我维持的巨大 H ⁺浓度差异的自发形成，这是连续发电的驱动力。此外，引入的具有最大电负性 (3.98) 的氟加速了羧基的电离并进一步放大了 H ⁺浓度差异。连接多个 H-OGF 设备可按比例放大高达 10 V 的电压，为电子设备供电并获得可穿戴电源。随着对位置或环境条件的严格要求放宽，我们的研究结果使 H-OGF 设备成为低预算和自我维持能源系统的有希望的候选者。