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온도 및 체류 시간 제어를 통한 메탄 열분해 수소 및 탄소 생성물 특성 연구

이문희1, 이상지2, 김지엽1, 주승엽3, 김륜근3, 남형석3, 홍정구3,#orcid

Hydrogen and Carbon Production via Methane Thermal Decomposition: Effects of Temperature and Residence Time

Mun Hee Lee1, Sang Ji Lee2, Ji Yeop Kim1, Seung Yeop Joo3, Ryun Geun Kim3, Hyungseok Nam3, Jung Goo Hong3,#orcid
Journal of the Korean Society for Precision Engineering 2026;43(4):371-377.
Published online: April 1, 2026

1경북대학교 대학원 기계공학과

2고등기술연구원 에너지환경 IT융합그룹

3경북대학교 기계공학부

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#Corresponding Author / E-mail: jghong70@knu.ac.kr, TEL: +82-53-950-6570
• Received: September 5, 2025   • Revised: November 3, 2025   • Accepted: December 3, 2025

Copyright © The Korean Society for Precision Engineering

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  • Methane thermal decomposition is a promising technology for producing CO2-free hydrogen. This study experimentally examines how temperature (1,000–1,400oC) and residence time affect methane decomposition in a ceramic tubular reactor. The results show that both the methane conversion rate and hydrogen yield increased with temperature, reaching approximately 95% and 45%, respectively, at 1,400oC. At lower temperatures (1,000–1,200oC), residence time had a significant impact, while at higher temperatures (1,300–1,400oC), temperature became the predominant factor. Additionally, the formation of C2 hydrocarbons, particularly acetylene (C2H2), increased as residence time decreased, negatively affecting both methane conversion and hydrogen yield. Analysis of the solid carbon by-products identified two distinct forms: amorphous, spherical carbon black particles and a semi-graphitic, crystalline carbon film. These findings provide essential data for optimizing the conditions of methane thermal decomposition.
  • KEYWORDS: Methane thermal decomposition, Hydrogen, Residence time, Conversion rate, Carbon products
  • KEYWORDS: 메탄 열분해, 수소, 체류 시간, 전환율, 탄소 생성물
전 세계적으로 기후변화에 대한 위기의식이 고조되고 있으며, 에너지 전환이 국가적, 산업적으로 가속화되고 있다[1]. 국제에 너지기구(IEA), 유럽연합(EU), 한국 등 주요 국가에서는 이산화탄소 배출량을 0이 되도록 하는 Net-zero 목표를 제시하고 있으며, 이에 따라서 기존의 화석연료 기반의 체계에서 새로운 에너지 체계로의 전환이 요구되고 있다[2]. 이 과정에서 수소는 기존의 화석연료를 대체 가능하며, 탈탄소 산업공정으로의 전환, 에너지 저장과 운송 등을 만족할 수 있는 차세대 에너지원으로 각광받고 있다[3].
현재 수소를 생산하는 방법에는 전기를 이용한 수전해, 화석 연료 개질, 열화학적 분해 등이 있으며, 생산하는 방법, 탄소 배출에 따라 회색, 블루, 그린, 청록수소로 나뉘게 된다[4]. 세계에 너지협의회에서 발표한 자료에 의하면 수소 생산의 96%가 화석연료의 개질을 통해 얻어지는 회색 수소이며, 단 4%만이 수전해를 통해 얻어지는 그린 수소이다[5]. 화석연료의 개질을 통해 얻어지는 회색 수소는 이산화탄소를 배출하기 때문에 장기적으로 활용하기 어렵다는 단점을 가지고 있다[4,5]. 이와 달리 그린 수소는 이산화탄소를 배출하지 않지만, 생산 단가가 높기 때문에 대량의 수소를 생산하기 어렵다는 단점을 가지고 있다[6].
이러한 단점을 보완할 수 있는 기술로서, 메탄 열분해 기술이 각광받고 있다[7]. 메탄 열분해 기술은 고온의 반응기에서 메탄을 분해하여 고체 탄소와 수소로 분해되므로, 이산화탄소를 배출하지 않는다. 고체 탄소는 타이어, 잉크, 전도성 소재 및 촉매 지지체 등에 활용될 수 있기 때문에 공정과정에서 경제성을 확보할 수 있다는 장점을 가지고 있다[8]. 또한 다른 수소 생산 기술에 비해 수소 에너지 소비 측면에서 장점을 가지고 있다[7,9].
그러나 메탄 열분해는 1,000°C 이상의 고온에서 반응이 시작되며, 고체 탄소로 인한 반응기의 막힘(Clogging)으로 연속적인 운전이 힘들다는 단점을 가지고 있다[10]. 이러한 단점을 해결하기 위해서 금속 촉매를 사용한 메탄 열분해, 유동층 반응기, 용융 금속을 사용한 열분해 등 다양한 연구가 진행되고 있다[11].
A. Aba´nades 등은 다공성 반응기 및 반응기 재질에 대한 연구를 수행하였으며, 반응기의 재질은 메탄 전환율에 영향을 미치지 않는다고 하였다. 또한 다공성 반응기에서도 탄소의 침착을 방지하지 못한다고 하였다[12]. Lee 등은 반응 온도에 따른 영향을 확인하였으며, 고온에서 수소의 선택도는 증가하지만, 고체 탄소로 인한 반응기 막힘으로 인해 지속시간이 짧아진다고 하였다. 또한 고온에서 메탄 열분해 반응이 모두 수소로 변환되는 것이 아닌 기타 탄화수소 계열로 전환되는 부반응이 동반된다고 하였다[13]. Tsegay Gebrekidan Gebreyohannes 등은 수치해석 기법을 활용하여 메탄 열분해 연구를 수행하였으며, 압력이 증가하면 기타 탄화수소의 탈수소화(Dehydrogenation) 반응이 억제되어 메탄 전환율이 감소한다고 하였다. 또한 온도와 압력이 전환율과 수율에 핵심적인 역할을 한다고 하였다[14]. 그러나 기존 연구들은 수치해석 기법을 활용하거나, 주로 반응기의 구조적 특성이나 단일 변수(온도, 압력)에 초점을 맞추었으며, C2 탄화수소 생성이 전환율 및 수소 수율에 미치는 영향에 대해서는 충분히 규명하지 않았다.
본 연구에서는 이러한 한계를 보완하기 위해 관형 반응기에서 반응 온도 및 체류 시간에 대한 C2 탄화수소의 생성 거동과 메탄 전환율, 수소 수율간의 상관관계를 실험적으로 확인하고자 한다.
또한, 메탄 열분해 과정에서 생성된 탄소 생성물(Carbon Products)인 카본 블랙(Carbon Black), 카본 필름(Carbon Film)에 대한 성상 및 결정성을 확인하고자 한다. 이는 향후에 메탄 열분해에 공정 설계 및 촉매를 사용한 열분해에 기초 데이터로 활용될 수 있을 것으로 판단된다.
2.1 실험 장치
Fig. 1은 메탄 열분해의 실험장치도를 나타낸다. 실험장치는 크게 유체 공급부, 반응부, 계측부로 나뉘어진다. 유체 공급부에서는 질량 유량 조절기(Mass Flow Controller, MFC)를 이용하여 메탄, 질소 가스를 공급하였으며, 반응기 전단에서 혼합된 후 반응기로 공급되었다. 반응부에서는 반응기와 가열장치로 구성되었으며, 반응기는 세라믹 재질로, 내경은 27 mm이며 길이는 1,000 mm이다. 가열장치는 최대 1,500°C까지 승온할 수 있는 전기 가열로를 사용하였다.
반응기는 전기 가열로에서 고온으로 유지되며, 반응기 중단에 있는 R-type 열전대(R-type Thermocouple)을 사용해서 온도를 확인하였다. 마지막으로 계측부에서는 메탄 열분해 반응으로부터 생성된 탄소 생성물을 포집하기 위해 세틀링 챔버(Settling Chamber)를 사용하였다. 포집된 탄소는 이후 결정구조를 확인하기 위해 X선 회절 분석(X-ray Diffraction Method, XRD)와 탄소의 형태를 확인하기 위해 주사전자현미경(Scanning Electron Microscope, SEM)로 분석하였다. 열분해로부터 생성된 가스는 가스 크로마토그래피(Gas Chromatography, GC)를 사용하여 분석하였으며, GC에서 분석하기 전에 세틀링 챔버에서 걸러지지 않은 탄소 생성물을 한 번 더 걸러주기 위해 팀블 필터(Thimble Filter)를 사용하였다. GC는 열전도도 검출기(Thermal Conductivity Detector, TCD)를 사용하여 수소, 메탄, 질소의 농도를 확인하였으며, 불꽃 이온화 검출기(Flame Ionization Detector, FID)를 사용하여 C2 탄화수소를 확인하였다.
2.2 실험 조건 및 실험 방법
Table 1은 메탄 열분해에서 온도 및 체류 시간에 대한 영향을 확인하기 위한 실험조건을 나타낸다. 실험에서 설정한 온도는 1,000-1,400°C이다. 반응기에서 공급되는 질소, 메탄의 분율(Fraction)을 고정한 채, Case에 따라 유량을 1-3 L까지 조정하면서 체류 시간에 따른 영향을 확인하였다. 반응기 내에서 유량이 증가함에 따라 체류 시간이 감소하며, 이는 반응기에서 메탄이 반응하는 시간에 영향을 미치기 때문에 변수 조건으로 설정하였다.
반응기에 질소로 퍼지(Purge)하면서 설정한 온도까지 승온시켰다. 이후 설정한 온도에 도달하면 메탄과 질소를 설정한 유량 만큼 공급하였다. 메탄 열분해 반응으로 생성된 가스는 GC를 이용해서 실시간으로 분석하였으며, 실험 결과는 총 실험 시간 동안의 값을 평균한 값이다. 또한 반응기 후단의 압력계 및 비커를 통해서 탄소 생성물에 의한 막힘을 확인하였다. 압력계를 통하여 1차적으로 반응기 후단 및 배관의 막힘을 확인하였으며, 비커에서 기포가 발생하지 않으면 반응기가 완전히 막혔다고 판단하였다.
GC를 통해 계측한 데이터를 가지고 다음의 수식을 이용해서 메탄 전환율, 수소 및 C2 탄화수소의 수율을 분석하였다. 식(1)은 메탄 전환율을 나타내며, FCH4, in와 FCH4, out는 반응 전후의 메탄의 유량을 의미한다. 식(2)와 식(3)은 수소 및 C2 탄화수소의 수율을 나타낸 식으로, 공급된 메탄 대비 생성된 수소, 탄화수소비로 계산되었다.
(1)
XCH4=(1-FCH4,outFCH4,in)×100
(2)
YH2=12×(FCH2,outFCH4,in)×100
(3)
YC2=2×(FC2,outFCH4,in)×100
3.1 메탄 전환율 및 수소 수율
Fig. 2는 온도 및 Case에 따른 메탄 전환율을 나타낸다. 모든 조건에서 온도가 증가함에 따라 메탄 전환율이 증가하는 것을 확인할 수 있다. 이는 메탄 열분해 반응이 흡열 반응이므로, 고온에서 열분해 반응이 활발하게 일어나며, 반응속도가 증가하기 때문이다.
유량 변화에 따른 메탄 전환율의 차이를 확인하면, 공급 유량이 증가함에 따라 메탄 전환율이 감소하는 것을 확인할 수 있다. 이는 공급 유량이 증가함에 따라 체류 시간이 감소하여 반응이 충분히 일어나지 못하기 때문에 메탄 전환율이 낮아진다. 또한, 반응 온도가 1,000-1,200°C에서는 체류 시간에 대한 영향이 큰 것을 확인할 수 있으며, 1,300-1,400°C에서는 반응 온도에 따른 영향이 지배적이며, 체류 시간에 대한 영향은 적은 것을 확인할 수 있다.
Fig. 3는 수소 수율을 나타낸 그래프로서, 앞선 메탄 전환율 결과와 유사하게 반응 온도가 증가함에 따라 수소 수율도 증가한다. 또한 동일한 온도에서 체류 시간이 길수록 수소 수율이 증가하는 것을 확인할 수 있다. 본 실험의 최고 온도에서 메탄 전환율은 약 94-95%로 확인되었으며, 이 때의 수소 수율은 약 44-45%로 나타내었다. 전환율과 수율만을 기준으로 평가했을 때, 이는 다른 기술에 비해 높은 수준을 나타낸다[11].
또한 메탄 전환율, 수소 수율 그래프를 통해 Lee 등의 연구에서와 동일하게 메탄이 모두 수소로 변환되지 않는 것을 확인할 수 있으며, 이를 확인하고자 C2 탄화수소의 수율을 확인하였다[13].
3.2 C2 탄화수소 수율
Fig. 4는 C2 탄화수소 아세틸렌(Acetylene, C2H2), 에틸렌(Ethylene, C2H4), 에탄(Ethane, C2H6)의 수율을 확인한 결과이다. 모든 조건에서 반응 온도가 증가함에 따라 아세틸렌, 에틸렌은 증가하는 경향을 보였다. 그러나 에탄의 경우 모든 조건에서 수율이 0에 수렴하는 것을 확인할 수 있다. 또한 공급 유량이 증가할수록, 즉 체류 시간이 짧아질수록 에탄, 에틸렌의 경우는 큰 차이가 없었으나 아세틸렌의 수율이 증가하는 것을 확인하였다.
이는 초기 메탄 열분해 반응에서 CH4 → CH3·+H·로 분해되어 CH3·, H· 라디칼(Radical)을 형성하게 되고, 라디칼의 재중합으로 인해 C2H6, H2가 생성된다. 이에 따라 제일 초기에 형성되는 에탄이 먼저 분해되어 모든 조건에서 수율이 0에 수렴하는 것으로 판단된다. 이후 반응과정에서 C2H6 → C2H4+H2로 전환되는 분해 과정을 거치게 되며, C2H4 → C2H2 +H2로 분해되는 과정을 거치게 된다. 이후 아세틸렌은 추가적인 반응을 통해 기타 탄화수소와 수소를 형성하게 된다. 체류 시간이 감소함에 따라 아세틸렌이 추가적인 반응이 일어나지 않아 Case 3에서 아세틸렌의 수율이 증가하는 것으로 판단되며, 이런 영향으로 체류 시간이 감소함에 따라 메탄 전환율 및 수소 수율이 감소하는 것으로 확인된다. Lee 등의 수치해석을 통한 메탄 열분해에서도 이와 같이 체류 시간이 짧을 때 비교적 저분자 탄화수소의 합성이 증가하여, 아세틸렌, 에틸렌 등이 증가한다고 하였으며, 이와 부합하는 결과이다[15]. 이를 통하여 실험적으로 C2 탄화수소가 전환율 및 수율에 미치는 영향에 대해 실험적으로 확인하였다.
3.3 카본블랙 및 카본필름 분석
메탄 열분해를 통해 생성된 탄소 생성물은 세틀링 챔버에서 획득하였으며, 카본 블랙(Carbon Black), 카본 필름(Carbon Film) 두 가지의 탄소 생성물을 획득하였다. Fig. 5는 카본 블랙 및 카본 필름의 원시 이미지(Raw Image)를 나타낸다. 탄소 생성물들의 형태 및 결정성을 확인하기 위하여 SEM, XRD 분석을 수행하였다.
Fig. 6는 카본 블랙의 SEM 이미지이다. SEM 이미지를 통하여 카본 블랙은 비교적 균일한 크기의 구형 입자들로 확인된다. 또한 카본 블랙의 직경은 대략 수십-수백 nm로 확인되었다. 또한 고배율에서 찍은 이미지를 통하여 카본 블랙 입자들이 서로 응집(Aggregate)되어 하나의 덩어리로 형성되는 것을 확인할 수 있다.
Fig. 7은 카본 필름의 SEM 이미지로서, 표면 중앙에 카본 블랙이 응집되어 덩어리가 형성되어 있는 구조를 확인할 수 있다. 카본 블랙이 응집되어 있는 곳과 표면을 확인한 결과, nm 크기의 카본 블랙이 응집되어 형성되어 있는 것을 확인할 수 있으며, 표면에서는 거칠고 불균일한 표면이 형성되는 것을 확인할 수 있다.
이를 통해서 먼저 형성된 카본 블랙이 반응기 표면에 침착(Deposition)되어 하나의 필름을 형성하고 필름의 표면 위의 카본 블랙이 응집되는 것으로 판단된다.
탄소 생성물의 결정성은 XRD 패턴을 통해서 확인하였으며, Fig. 8은 탄소 생성물들의 XRD 패턴을 나타낸다. 먼저 카본 블랙의 경우 넓고 완만한 패턴이 확인되며, 피크가 뚜렷하지 않은 것을 확인할 수 있다. 이를 통해 비정질(Amorphous) 구조를 가지고 있는 카본 블랙임을 확인할 수 있다. 이와 달리, 카본 필름의 XRD 패턴에서는, 약 26°에서 특징적인 피크가 확인되며 결정성을 갖고 있는 것으로 판단된다. Mehran Dadsetan 등의 연구에서 카본 필름에 대한 분석을 수행하였으며, 반흑연 구조(Semi-graphitic Structure)를 가지고 있으며, 전도성이 높다고 하였다[16,17]. 탄소 생성물의 결정성과 형상을 확인함으로써, 메탄 열분해 과정에서 생성된 탄소 생성물들을 타이어, 잉크, 전도성 소재 등과 같은 산업에서 활용할 수 있는 기초 데이터를 제공할 수 있을 것으로 기대한다.
본 연구에서는 메탄 열분해 실험을 수행하여 반응 온도 및 체류 시간이 메탄 전환율, 수소 수율에 미치는 영향에 대해 확인하였으며, 탄소 생성물의 성상 및 결정성을 확인하였다. 주요 결론은 다음과 같다.
메탄 전환율과 수소 수율에 대한 온도와 체류 시간의 영향이 온도 구간에 따라 다르게 작용함을 확인하였다. 1,300°C 이상의 고온 영역에서는 온도가 반응을 지배하는 핵심 인자였으나, 1,200°C 이하의 저온 영역에서는 체류 시간의 영향이 지배적으로 나타났다. 이는 고효율 공정 설계 시 에너지 투입과 반응기 크기 등 운전 조건을 최적화하기 위해 온도 구간별로 주요 제어 변수를 다르게 설정해야 함을 시사한다.
C2 탄화수소를 부산물이 수소 수율을 저해하는 핵심 요인임을 실험적으로 확인하였다. 체류 시간이 짧아질수록 아세틸렌(C2H2)과 같은 2차 반응물의 생성이 증가하며, 이것이 메탄의 완전한 분해 반응을 저해하여 전체 수소 수율을 감소시키는 주요 원인으로 작용함을 확인하였다.
메탄 열분해로부터 생성된 탄소 생성물은 카본 필름, 카본 블랙 두 가지의 형태로 확인되었으며, 카본 블랙은 구형 입자가 응집된 형태로 확인되었다. 카본 필름은 표면이 불균일한 형태를 가지며 카본 블랙이 응집된 영역이 확인되었다. 또한 XRD 분석을 통해 카본 필름은 결정성을 가지고 있는 것을 확인하였다.
Fig. 1
Schematic diagram of methane thermal decomposition experimental apparatus
JKSPE-025-130f1.jpg
Fig. 2
Conversion rate of CH4 to temperature & case
JKSPE-025-130f2.jpg
Fig. 3
Hydrogen yield to temperature & case
JKSPE-025-130f3.jpg
Fig. 4
C2 hydrocarbon yield to temperature & case
JKSPE-025-130f4.jpg
Fig. 5
Carbon black (Left) & carbon film (Right)
JKSPE-025-130f5.jpg
Fig. 6
SEM image of carbon black
JKSPE-025-130f6.jpg
Fig. 7
SEM image of carbon film
JKSPE-025-130f7.jpg
Fig. 8
XRD spectra of the carbon black, carbon film
JKSPE-025-130f8.jpg
Table 1
Experimental conditions
Table 1
Case Temperature [°C] CH4 flowrate [LPM] N2 flowrate [LPM]
Case 1 1,000–1,400 1 1
Case 2 2 2
Case 3 3 3
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Mun Hee Lee
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Ph.D. candidate in the Department of Mechanical Engineering, Kyungpook National University. His research interest is thermal decomposition.
Sang Ji Lee
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Senior researcher in the Department of Energy Environment IT Convergence Group, Institute for Advanced Engineering. His research interest is bio-char/torrefaction and biomass plant demonstration
Ji Yeop Kim
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Ph.D. in the Department of Mechanical Engineering, Kyungpook National University. His research interest is electrospray.
Seung Yeop Joo
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B.Sc. candidate in the Department of Mechanical Engineering, Kyungpook National University. His research interest is thermal decomposition.
Ryun Geun Kim
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B.Sc. candidate in the Department of Mechanical Engineering, Kyungpook National University. His research interest is thermal decomposition.
Hyungseok Nam
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Professor in the Department of Mechanical Engineering, Kyungpook National University. His research interest is carbon neutral energy conversion, CO2 capture/utilization and thermal fluid system.
Jung Goo Hong
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Professor in the Department of Mechanical Engineering, Kyungpook National University. His research interest is combustion engineering, atomization and spray.

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Hydrogen and Carbon Production via Methane Thermal Decomposition: Effects of Temperature and Residence Time
J. Korean Soc. Precis. Eng.. 2026;43(4):371-377.   Published online April 1, 2026
DOI: https://doi.org/10.7736/JKSPE.025.130
Download Citation

Download a citation file in RIS format that can be imported by all major citation management software, including EndNote, ProCite, RefWorks, and Reference Manager.
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Hydrogen and Carbon Production via Methane Thermal Decomposition: Effects of Temperature and Residence Time
J. Korean Soc. Precis. Eng.. 2026;43(4):371-377.   Published online April 1, 2026
DOI: https://doi.org/10.7736/JKSPE.025.130
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Hydrogen and Carbon Production via Methane Thermal Decomposition: Effects of Temperature and Residence Time
Image Image Image Image Image Image Image Image
Fig. 1 Schematic diagram of methane thermal decomposition experimental apparatus
Fig. 2 Conversion rate of CH4 to temperature & case
Fig. 3 Hydrogen yield to temperature & case
Fig. 4 C2 hydrocarbon yield to temperature & case
Fig. 5 Carbon black (Left) & carbon film (Right)
Fig. 6 SEM image of carbon black
Fig. 7 SEM image of carbon film
Fig. 8 XRD spectra of the carbon black, carbon film

Fig. 1

Fig. 2

Fig. 3

Fig. 4

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Fig. 8

Hydrogen and Carbon Production via Methane Thermal Decomposition: Effects of Temperature and Residence Time
Case Temperature [°C] CH4 flowrate [LPM] N2 flowrate [LPM]
Case 1 1,000–1,400 1 1
Case 2 2 2
Case 3 3 3
Table 1 Experimental conditions

Table 1

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