Chloride-Engineered CO Selectivity Promotion in Integrated Carbon Capture and Hydrogenation
Achieving high CO selectivity in integrated carbon capture and hydrogenation (ICCH) remains a challenge because Ni-based dual functional materials (DFMs) inevitably catalyze competing methanation. Here, we demonstrate that trace chloride incorporation into Ni–Ca DFMs switches the dominant hydrogenation pathway from methanation to the reverse water−gas shift reaction. Chloride preferentially interacts with the CaO sorbent phase, forming Ca–Cl species that drive CaO densification and substantially lower the reducibility of the adjacent Ni active sites. Consequently, the 1% Cl-modified DFM attains 91.6% CO selectivity at 600 °C, in contrast to the 20.5% CO selectivity of the Cl-free counterpart. Cyclic testing confirms that the Cl-modified DFM maintains stable CO 2 conversion and high CO selectivity. In situ experiments further show that chloride suppresses the deep hydrogenation of formate intermediates, thereby terminating the reaction at the CO-forming step rather than proceeding to CH 4 . This study establishes halogen engineering as an effective and operationally simple strategy for steering product selectivity in ICCH processes.
Authors
- Shuzhuang Sun (ORCID: https://orcid.org/0000-0003-1573-8713)
- Yaozu Wang (ORCID: https://orcid.org/0000-0002-4392-6634)
- Yanguo Zhang (ORCID: https://orcid.org/0000-0002-2343-6427)
- Hui Zhou (ORCID: https://orcid.org/0000-0003-1410-4794)
- Hailong Zhang (ORCID: https://orcid.org/0000-0002-8951-7094)
- Haiyang Liu (ORCID: https://orcid.org/0000-0001-9236-4490)
- Xiaohan Li (ORCID: https://orcid.org/0000-0001-9493-3597)
- Qinghai Li (ORCID: https://orcid.org/0000-0002-5300-9629)
- Wentao Du (ORCID: https://orcid.org/0000-0003-1848-646X)
- Bocheng Yu (ORCID: https://orcid.org/0000-0001-6482-6985)
- Shaoguang Feng
- Dingli Li
- Muqing Yang
- Fangjing Du
- Xuan Bie
- Yijian Qiao
Institutions
- Zhengzhou University (CN)
- Ministry of Education (RO)
- Huaneng Clean Energy Research Institute (CN)
- Datang Telecom Group (China) (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- ACS Sustainable Chemistry & Engineering
- Published
- 2026-06-26
- DOI
- https://doi.org/10.1021/acssuschemeng.6c04179
- Primary Topic
- Catalysts for Methane Reforming
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Ministry of Science and Technology of the People's Republic of China
- Tsinghua University
- Natural Science Foundation of Shanxi Province
- Natural Science Foundation of Henan Province
- Shanxi Research Institute for Clean Energy
- Hebei Province Science and Technology Support Program