High Yield of CO and Synchronous S Recovery from the Conversion of CO2 and H2S in Natural Gas Based on a Novel Electrochemical Reactor

被引:27
作者
Zhang, Bo [1 ]
Bai, Jing [1 ]
Zhang, Yan [1 ]
Zhou, Changhui [1 ]
Wang, Pengbo [1 ]
Zha, Lina [1 ]
Li, Jinhua [1 ]
Simchi, Abdolreza [2 ]
Zhou, Baoxue [1 ,3 ]
机构
[1] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Key Lab Thin Film & Microfabricat Technol, Minist Educ, Shanghai 200240, Peoples R China
[2] Sharif Univ Technol, Dept Mat Sci & Engn, Tehran 1458889694, Iran
[3] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
基金
中国国家自然科学基金;
关键词
H2S splitting; CO2; conversion; natural gas purification; synchronous recovery of S and CO; HYDROGEN-SULFIDE; SIMULTANEOUS ABSORPTION; ACID GASES; REDUCTION; REMOVAL; ELECTRODE; MEMBRANE; ELECTROREDUCTION; DECOMPOSITION; SYSTEMS;
D O I
10.1021/acs.est.1c04414
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
H2S and CO2 are the main impurities in raw natural gas, which needs to be purified before use. However, the comprehensive utilization of H2S and CO2 has been ignored. Herein, we proposed a fully resource-based method to convert toxic gas H2S and greenhouse gas CO2 synchronously into CO and elemental S by using a novel electrochemical reactor. The special designs include that, in the anodic chamber, H2S was oxidized rapidly to S based on the I-/I-3(-) cyclic redox system to avoid anode passivation. On the other hand, in the cathodic chamber, CO2 was rapidly and selectively reduced to CO based on a porous carbon gas diffusion electrode (GDE) modified with polytetrafluoroethylene and cobalt phthalocyanine (CoPc). A high Faraday efficiency (>95%) toward CO was achieved due to the enhanced mass transfer of CO2 on the GDE and the presence of the selective CoPc catalyst. The maximum energy efficiency of the system was more than 72.41% with a current density of over 50 mA/cm(2), which was 12.5 times higher than what was previously reported on the H2S treatment system. The yields of S and CO were 24.94 mg.cm(-2).h(-1) and 19.93 mL.cm(-2).h(-1), respectively. A model analysis determined that the operation cost of the synchronous utilization of H2S and CO2 method was slightly lower than that of the single utilization of H2S in the existing natural gas purification technology. Overall, this paper provides efficient and simultaneous conversion of H2S and CO2 into S and CO.
引用
收藏
页码:14854 / 14862
页数:9
相关论文
共 56 条
[1]   Zinc-Modified Copper Catalyst for Efficient (Photo-)Electrochemical CO2 Reduction with High Selectivity of HCOOH Production [J].
Ajmal, Saira ;
Yang, Yang ;
Li, Kejian ;
Tahir, Muhammad Ali ;
Liu, Yangyang ;
Wang, Tao ;
Bacha, Aziz-Ur-Rahim ;
Feng, Yiqing ;
Deng, Yue ;
Zhang, Liwu .
JOURNAL OF PHYSICAL CHEMISTRY C, 2019, 123 (18) :11555-11563
[2]   ELECTROCHEMICAL PRODUCTION OF HYDROGEN AND SULFUR BY LOW-TEMPERATURE DECOMPOSITION OF HYDROGEN-SULFIDE IN AN AQUEOUS ALKALINE-SOLUTION [J].
ANANI, AA ;
MAO, Z ;
WHITE, RE ;
SRINIVASAN, S ;
APPLEBY, AJ .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (09) :2703-2709
[3]   Preparation of a Pb loaded gas diffusion electrode and its application to CO2 electroreduction [J].
Ang Li ;
Hua Wang ;
Jinyu Han ;
Li Liu .
Frontiers of Chemical Science and Engineering, 2012, 6 (4) :381-388
[4]   Effect of pore structure and surface chemistry of virgin activated carbons on removal of hydrogen sulfide [J].
Bandosz, TJ .
CARBON, 1999, 37 (03) :483-491
[5]   Hybrid processes for the removal of acid gases from natural gas [J].
Bhide, BD ;
Voskericyan, A ;
Stern, SA .
JOURNAL OF MEMBRANE SCIENCE, 1998, 140 (01) :27-49
[6]   Review of gas diffusion cathodes for alkaline fuel cells [J].
Bidault, F. ;
Brett, D. J. L. ;
Middleton, P. H. ;
Brandon, N. P. .
JOURNAL OF POWER SOURCES, 2009, 187 (01) :39-48
[7]   A Local Proton Source Enhances CO2 Electroreduction to CO by a Molecular Fe Catalyst [J].
Costentin, Cyrille ;
Drouet, Samuel ;
Robert, Marc ;
Saveant, Jean-Michel .
SCIENCE, 2012, 338 (6103) :90-94
[8]   Application of cobalt phthalocyanine as a nanostructured catalyst in the synthesis of biological henna-based compounds [J].
Dashteh, Mohammad ;
Safaiee, Maliheh ;
Baghery, Saeed ;
Zolfigol, Mohammad Ali .
APPLIED ORGANOMETALLIC CHEMISTRY, 2019, 33 (04)
[9]   What would it take for renewably powered electrosynthesis to displace petrochemical processes? [J].
De Luna, Phil ;
Hahn, Christopher ;
Higgins, Drew ;
Jaffer, Shaffiq A. ;
Jaramillo, Thomas F. ;
Sargent, Edward H. .
SCIENCE, 2019, 364 (6438) :350-+
[10]   Insights on natural gas purification: Simultaneous absorption of CO2 and H2S using membrane contactors [J].
Faiz, Rami ;
Al-Marzouqi, M. .
SEPARATION AND PURIFICATION TECHNOLOGY, 2011, 76 (03) :351-361